WO2008007886A1 - Fuel cell separator using the graphite composite and preparing method thereof - Google Patents
Fuel cell separator using the graphite composite and preparing method thereof Download PDFInfo
- Publication number
- WO2008007886A1 WO2008007886A1 PCT/KR2007/003331 KR2007003331W WO2008007886A1 WO 2008007886 A1 WO2008007886 A1 WO 2008007886A1 KR 2007003331 W KR2007003331 W KR 2007003331W WO 2008007886 A1 WO2008007886 A1 WO 2008007886A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- graphite
- powder
- composite
- fuel cell
- tamping
- Prior art date
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 77
- 239000002131 composite material Substances 0.000 title claims abstract description 74
- 229910002804 graphite Inorganic materials 0.000 title claims abstract description 51
- 239000010439 graphite Substances 0.000 title claims abstract description 51
- 239000000446 fuel Substances 0.000 title claims abstract description 48
- 238000000034 method Methods 0.000 title claims description 19
- 239000000843 powder Substances 0.000 claims abstract description 41
- 238000004519 manufacturing process Methods 0.000 claims abstract description 34
- 229920001187 thermosetting polymer Polymers 0.000 claims abstract description 18
- 238000001035 drying Methods 0.000 claims abstract description 17
- 239000005011 phenolic resin Substances 0.000 claims abstract description 17
- 239000003822 epoxy resin Substances 0.000 claims abstract description 11
- 229920000647 polyepoxide Polymers 0.000 claims abstract description 11
- 239000004848 polyfunctional curative Substances 0.000 claims abstract description 11
- 239000006185 dispersion Substances 0.000 claims description 14
- 229910021382 natural graphite Inorganic materials 0.000 claims description 9
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 4
- 239000000654 additive Substances 0.000 claims description 4
- 239000004917 carbon fiber Substances 0.000 claims description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 4
- 239000006229 carbon black Substances 0.000 claims description 3
- 238000005452 bending Methods 0.000 claims 1
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 abstract description 12
- 239000002904 solvent Substances 0.000 abstract description 8
- 229920005989 resin Polymers 0.000 abstract description 5
- 239000011347 resin Substances 0.000 abstract description 5
- 239000004634 thermosetting polymer Substances 0.000 abstract description 5
- 239000012528 membrane Substances 0.000 abstract description 3
- 238000000926 separation method Methods 0.000 abstract description 3
- 239000004593 Epoxy Substances 0.000 abstract description 2
- 239000005518 polymer electrolyte Substances 0.000 abstract description 2
- 230000000052 comparative effect Effects 0.000 description 9
- 239000000203 mixture Substances 0.000 description 8
- ZWEHNKRNPOVVGH-UHFFFAOYSA-N 2-Butanone Chemical compound CCC(C)=O ZWEHNKRNPOVVGH-UHFFFAOYSA-N 0.000 description 5
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 3
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 3
- 230000000996 additive effect Effects 0.000 description 3
- 238000007796 conventional method Methods 0.000 description 3
- 238000001816 cooling Methods 0.000 description 3
- 229910021383 artificial graphite Inorganic materials 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 239000011231 conductive filler Substances 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- QIVUCLWGARAQIO-OLIXTKCUSA-N (3s)-n-[(3s,5s,6r)-6-methyl-2-oxo-1-(2,2,2-trifluoroethyl)-5-(2,3,6-trifluorophenyl)piperidin-3-yl]-2-oxospiro[1h-pyrrolo[2,3-b]pyridine-3,6'-5,7-dihydrocyclopenta[b]pyridine]-3'-carboxamide Chemical compound C1([C@H]2[C@H](N(C(=O)[C@@H](NC(=O)C=3C=C4C[C@]5(CC4=NC=3)C3=CC=CN=C3NC5=O)C2)CC(F)(F)F)C)=C(F)C=CC(F)=C1F QIVUCLWGARAQIO-OLIXTKCUSA-N 0.000 description 1
- HFGHRUCCKVYFKL-UHFFFAOYSA-N 4-ethoxy-2-piperazin-1-yl-7-pyridin-4-yl-5h-pyrimido[5,4-b]indole Chemical compound C1=C2NC=3C(OCC)=NC(N4CCNCC4)=NC=3C2=CC=C1C1=CC=NC=C1 HFGHRUCCKVYFKL-UHFFFAOYSA-N 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000002041 carbon nanotube Substances 0.000 description 1
- 229910021393 carbon nanotube Inorganic materials 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 229910003460 diamond Inorganic materials 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 239000003273 ketjen black Substances 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 239000002113 nanodiamond Substances 0.000 description 1
- XULSCZPZVQIMFM-IPZQJPLYSA-N odevixibat Chemical compound C12=CC(SC)=C(OCC(=O)N[C@@H](C(=O)N[C@@H](CC)C(O)=O)C=3C=CC(O)=CC=3)C=C2S(=O)(=O)NC(CCCC)(CCCC)CN1C1=CC=CC=C1 XULSCZPZVQIMFM-IPZQJPLYSA-N 0.000 description 1
- 210000003254 palate Anatomy 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 238000010079 rubber tapping Methods 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0204—Non-porous and characterised by the material
- H01M8/0221—Organic resins; Organic polymers
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0204—Non-porous and characterised by the material
- H01M8/0213—Gas-impermeable carbon-containing materials
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0204—Non-porous and characterised by the material
- H01M8/0223—Composites
- H01M8/0226—Composites in the form of mixtures
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/10—Fuel cells with solid electrolytes
- H01M2008/1095—Fuel cells with polymeric electrolytes
-
- Y—GENERAL 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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
-
- Y—GENERAL 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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Definitions
- the present invention relates to separation plate of a Polymer Electrolyte
- Membrane Fuel Cell or Direct Methanol Fuel Cell made graphite composite mixed spheroidized graphite powder and thermoset powder in the dry process and tamping graphite composite to mold variably and forming compressively and hardening.
- Electrolyte Membrane Fuel Cell or Direct Methanol Fuel Cell made graphite composite mixed nodular graphite powder fabricated mechanically from needle graphite or plate graphite and thermoset powder such as phenol resin or epoxy resin in the dry process not to be used solvent and variably tamping graphite composite to mold patterned path and forming compressively by press and hardening.
- Said phenol resin is used powder type including hardener and Said epoxy is used for mixing resin powder and hardener.
- the fuel cell separator have high electrical couductivity and high elastic modulus and high precision size.
- Fig 3. is a isometric drawing of fuel cell separator
- the present invention provide a separator made graphite composite mixed spheroidized graphite powder and themoset powder in the dry process and tamping graphite composite to mold variably and forming compressively and hardening in dry oven.
- mean diameter of spheroidized graphite powder is lower than 10 ⁇ m the fluidity of powder become worse and time If mean diameter of spheroidized graphite powder is higher than 100 ⁇ m the manufacturing of separator is not easy. So mean diameter of spheroidized graphite powder is to be controlled at lO ⁇ m -lOO ⁇ rn. And spheroidized index is maintained over of 0.5 because in case of below of 0.5 the fluidity is not good.
- the ratio of natural graphite powder is 70 wt.% -95 wt.%, thermoset powder is 5 wt.% -30 wt.%.
- the apparent density of graphite powder and thermoset powder is at 0.5 to 1.0 g/cm so uniform mixture is possible in mixture mixer. And mixture of graphite powder and thermoset powder are uniform so fuel cell separator have good electric conductivity and good elastic modulus. In this time If the apparent density of graphite powder and thermoset powder is below than 0.5 g/cm the fluidity is bad and If said apparent density is high than 1.0 g/cm Dthe manufacturing of powder is not easy.
- dispersion of thickness is higher than ⁇ 30 ⁇ m electrical resistance is increased because of fail to contacting and the leakage of gas is grow up. Therefore to make sure of good contacting dispersion of thickness have to be lower than ⁇ 30. And to align of dispersion of thickness composite is tamped variably in grooved part and non grooved part. So dispersion of thickness of molded article is not higher than ⁇ 30 ⁇ m
- the pressure of forming is 1.0 ⁇ 5.0 kgf/cm .
- the molded articles is inserted between porous ceramic plate and porous metal plate so molded ratircles is not deformed.
- the temperature of hardening is 100 0 C ⁇ 200 0 CD, more desirable the temperature of hardening is 15O 0 C ⁇ 18O 0 C.
- the time of hardening is 10 ⁇ 100 minutes. So thermoset resin is dispersed uniformly in molded articles.
- the fuel cell electrical conductivity is 100 - 275 S/cm and elastic modulus is 40 ⁇ 55 MPa
- the present invention is fuel cell separator and manufacturing method, described below comparative and example.
- the composite is mixed 90 wt.% graphite power and
- dry type mixer is super mixer, Hentschel mixer, weightlessness mixer.
- Example 4 The separator manufactured as Example 4, At manufacturing of separator the composite is mixed 85 wt.% graphite power and 13.5 wt.% epoxy resin powder and hardener 1.5 wt.% [52] Example ⁇
- Example 7 The separator manufactured as Example 4, At manufacturing of separator the composite is mixed 80 wt.% graphite power and 18 wt.% epoxy resin powder and hardener 2 wt.% [54] Example7
- the composite is mixed 85.5 wt.% spheroidized graphite powder and 4.0 wt.% granulized carbon fiber and Ketjen Black 0.5 wt.% and
- the total quantity of composit is 100 wt. % which ratio of composite is mixed 90 wt.% graphite power and 10 wt.% phenol resin powder in wet process and the quantity of solvent methyl ethyl ketone 150 wt.% and the composite to be mixed in 5O 0 C at 5hr and the composite is mixed in mixer and tamped mold variably and formed in normal temperature at compressed pressure.
- Comparative 3 is the separator manufactured as Example 1, the separator is tamped mold uniformly and formed in normal temperature at compressed pressure [64] Comparative 4
- Comparative 4 is the separator manufactured as Example 4, the separator is tamped mold uniformly and formed in normal temperature at compressed pressure [66] Table 1 is showing formability, electric conductivity and elastic modulus of
- Table 2 is showing dispersion of thickness manufactured fuel cell separator by
- graphite composite fuel cell separator of the present invention is gaining time to shorten the time of forming to manufacture of graphite composite mixing spheroidized graphite powder and thermoset resin powder having similar apparent density.
- the graphite composite fuel cell separator of the present invention have good electrical conductivity higher than 100 S/cm and good elastic modulus higher than 40
- the graphite composite fuel cell separator of the present invention have efficiency and safety to have size precision of dispersion of separator thickness to below ⁇ 30 ⁇ m to tamp variably along to path [73]
- the graphite composite fuel cell separator of the present invention is saving time to form because mold is possible to form not necessary to heat and to cool.
Abstract
The present invention more particularly relates to separation plate of a Polymer Electrolyte Membrane Fuel Cell or Direct Methanol Fuel Cell made graphite composite mixed nodular graphite powder fabricated mechanically from needle graphite or plate graphite and thermoset powder such as phenol resin or epoxy resin in the dry process not to be used solvent and variably tamping graphite composite to mold patterned path and forming compressively by press and hardening. Said phenol resin is used powder type including hardener and Said epoxy is used for mixing resin powder and hardener. The fuel cell separator have high electrical couductivity and high elastic modulus and high precision size. As described above, graphite composite fuel cell separator of the present invention is gaining time to shorten the time of forming to manufacture of graphite composite mixing spheroidized graphite powder and thermoset resin powder having similar apparent density.
Description
Description
FUEL CELL SEPARATOR USING THE GRAPHITE COMPOSITE AND PREPARING METHOD THEREOF
Technical Field
[1] The present invention relates to separation plate of a Polymer Electrolyte
Membrane Fuel Cell or Direct Methanol Fuel Cell made graphite composite mixed spheroidized graphite powder and thermoset powder in the dry process and tamping graphite composite to mold variably and forming compressively and hardening.
[2] The present invention more particularly relates to separation plate of a Polymer
Electrolyte Membrane Fuel Cell or Direct Methanol Fuel Cell made graphite composite mixed nodular graphite powder fabricated mechanically from needle graphite or plate graphite and thermoset powder such as phenol resin or epoxy resin in the dry process not to be used solvent and variably tamping graphite composite to mold patterned path and forming compressively by press and hardening. Said phenol resin is used powder type including hardener and Said epoxy is used for mixing resin powder and hardener. The fuel cell separator have high electrical couductivity and high elastic modulus and high precision size. Background Art
[3] The conventional fuel cell separator is made as Fig.l. and is as follows.
[4] The composite is manufactured in mixing thermoset such as phenol resin or epoxy resin and conductive filler such as needle graphite, flake graphite, artificial graphite, expanded graphite, carbon black, carbon fiber, carbon nano tube or diamond light carbon in dry process. And the compound is deposited solvent icluding 80-120% methyl ethyl keton(MEK), isopropyl alcohol, methanol, acetone. And the composite is dried to remove solvent and granulized. This granulized composite is filled to mold to be heated and result in fuel cell separator(30).
[5] As such described, forming material and manufacturing method of fuel cell separator is disclosed in Japanese patent publication No. 2005-116335
[6] However as described conventional manufacturing method of fuel cell separator mixed conductive filler which is flake graphite or artificial graphite and thermoset compound in wet process. If the quantity of solvent is too small the composite is not dispersed sufficiently because of law viscosity of thermoset, and If the quantity of solvent is too large the composite the composite is to be sinked because of high viscosity of thermoset. Therefore fuel cell separator has poor electric conductivity and poor elastic modulus. And the conductivity is to be curtailed as to lengthen of volatilizing time and manufacturing cost of additional facilities of recycling solvent.
[7] The bipolar plate and manufacturing method of fuel cell separator is disclosed in
Japanese patent publication No. 2004-338269. this method is mixing graphite powder and low- viscosity thermoset in liquid state and tamping composite to mold and heating mold and compressing in prescribed pressure and separating composite from mold and cooling the composite. This method is to be curtailed conductivity because the time of heating and cooling of mold from minmimum 9 minutes to maximum 20 minutes. So worker have to prepare two mold and preheater and additional cooling system and the cost is increased.
[8] In case Molded article is separated from mold not to be enough cooled state, the molded articles are deformed and dispersion of thickness is growing up and size precision is lowered and the fuel is to be leak after assembling.
[9] In case of forming of fuel cell separator(300) illustrated in Fig 3, dispersion of thickness grooved part(301) described dot line and non-grooved part(302) is growing up in state tamped same pressure of 0.5 - 1.0 g/cm illustrated in Fig 4. The dispersion of inner part and outer part of grooved part is growing up to be bulged in the center part. And If there is used this separator, it is contacted to Gas Diffusion Layer(GDL) non-uniformly and it is to be leaked after assembling. In characteristic of fuel cell separator this separator is not satisfied in requirement US DOE (Department of Energy) have small dispersion of thickness and have lower than 100 S/cm in electric conductivity and higher than 40MPa in elastic modulus Disclosure of Invention
Technical Problem
[10] It is, therefore, an object of the present invention to solved problems of conventional technical as described.
[11] It is also an abject of the present invention to provide graphite composite and the same method having lower than 100 S/cm in electric conductivity and higher than 40MPa in elastic modulus to be request by DOE
[12] It is also an abject of the present invention to provide graphite composite and the same method to simplify of manufacturing for molded article as to manufacturing of graphite composite to mix uniformly in dry process. To satisfy this object graphite composite is mechanically fabricated from natural graphite such as DD graphite or DD graphite and is mixed with phenol resin powder including hardener or epoxy resin power.
[13] It is also an abject of the present invention to provide graphite composite and the same method to have good electric conductivity and elastic modulus to manufacture fuelcell separator to harden for prescribed time and in higher temperature range from about 10 to 40 0C than hardening temperature of epoxy resin or phenol resin in drying
oven.
[14] It is also an abject of the present invention to provide graphite composite and the same method to have low dispersion of thickness and good size precision in grooved part and non-grooved part after forming to tamp differently each part. Brief Description of the Drawings
[15] Fig 1. is a flow chart of the conventional method of fuel cell separator
[16] Fig 2. is a flow chart of manufacturing fuel cell separator using composite.
[17] Fig 3. is a isometric drawing of fuel cell separator
[18] Fig 4. is a drawing of showing of conventional uniform tamping
[19] Fig 5. is a sectional view of fuel cell separator after forming compressively in conventional method illustrated in Fig 4.
[20]
[21] *Fig 6. is a drawing of stamping state of the present invention
[22] Fig 7. is a sectional view of fuel cell separator after forming compressively in variable tamping of the present invention.
[23] < explain of number of importance in drawings >
[24] 100 : manufacturing method of composite 200 : forming and hardening process
[25] 300 : fuel cell separator 301 : grooved part
[26] 302 : non grooved part
Best Mode for Carrying Out the Invention
[27] The present invention provide a separator made graphite composite mixed spheroidized graphite powder and themoset powder in the dry process and tamping graphite composite to mold variably and forming compressively and hardening in dry oven.
[28] The present invention will be described in more details as follows.
[29] Fig 2. is an flow chart of manufacturing fuel cell separator using composite and Fig
3. is isometric drawing of fuel cell separator and Fig 4. is drawing of showing of conventional uniform tamping and Fig 5. is sectional view of fuel cell separator after forming compressively in conventional method illustrated in Fig 4. and Fig 6. is drawing of stamping state of the present invention and Fig 7. is sectional view of fuel cell separator after forming compressively in variable tamping of the present invention.
[30] Therefore the present invention comprise 4 step including 2 stage to manufacturing of composite and 2 stage to form and to harden of composite
[31] In the manufacturing of composite for fuel cell separator, using of graphite spheroidizing of needle or palate graphite having mean mesh of powder at 10 to 100 μm and spheroidizing index at 0.5 to 1.0 and apparent density at 0.5 to 1.0 g/cm . Therefore the anisotropy of the composite is lower and equalization of electric con-
ductivity in radial direction and plate direction is grow up and equalization of resin powder is improved, so the powder is tamped uniformly so as to elevate of fluidity. At this time If mean diameter of spheroidized graphite powder is lower than 10 μm the fluidity of powder become worse and time If mean diameter of spheroidized graphite powder is higher than 100 μm the manufacturing of separator is not easy. So mean diameter of spheroidized graphite powder is to be controlled at lOμm -lOOμrn. And spheroidized index is maintained over of 0.5 because in case of below of 0.5 the fluidity is not good.
[32] The thermoset reisn such as the phenol resin and epoxy resin is to be mixed with spheroidized graphite powder to mix uniformly. Phenol resin is used with implying hardener and expox resin is used mixture with hardener. Said the mean diameter of thermoset resin is at 10 ~ 150 D so as to similar with diameter of graphite powder.
[33] The mixture ratio of natural graphite powder and theremoset powder is 70:30 ~
95:5. If the mixture ratio is over 30% electric resistance is raised so electric conductivity is not good and If the mixture ratio is below 5% is not enough adhere so the mechanical strength is not good.
[34] Therefore the ratio of natural graphite powder is 70 wt.% -95 wt.%, thermoset powder is 5 wt.% -30 wt.%. As described, the apparent density of graphite powder and thermoset powder is at 0.5 to 1.0 g/cm so uniform mixture is possible in mixture mixer. And mixture of graphite powder and thermoset powder are uniform so fuel cell separator have good electric conductivity and good elastic modulus. In this time If the apparent density of graphite powder and thermoset powder is below than 0.5 g/cm the fluidity is bad and If said apparent density is high than 1.0 g/cm Dthe manufacturing of powder is not easy.
[35] In case of mixture uniformly natural graphite powder and thermoset resin powder in dry process to improve mechanical strength and electrical conductivity in fuel cell separator can contain additive contain carbon fiber or carbon black 1 wt.% - 5.0 wt.%. If the ratio of said additive is high than 5.0 wt.% material cost is high so the ratio of additive is at 0.1 wt.% to 5.0 wt.%
[36] In the manufacturing of fuel cell separator composite as described is tamped to mold. To minimize of diversion of thickness and to improve of size precision the composite is to be tamped varailblt which tamped 0.8 - 1.2 g/cm in apparent density at non grooved part and tamped 0.5 - 1.0 g/cm In apparent at grooved part. So the forming density is to be unique and the separator have small dispersion of thickness and high size precision to ± 30 μm as to outer part and groove of separator as illustrated in Fig 7. In this time variable tamping is unbalanced gas tapping or multi- layered powder tamping. The tamping density is unique wholly and dispersion of thickness ± 30 μm. If dispersion of thickness is higher than ± 30 μm electrical
resistance is increased because of fail to contacting and the leakage of gas is grow up. Therefore to make sure of good contacting dispersion of thickness have to be lower than ± 30. And to align of dispersion of thickness composite is tamped variably in grooved part and non grooved part. So dispersion of thickness of molded article is not higher than ± 30 μm
[37] The pressure of forming is 1.0 ~ 5.0 kgf/cm . The molded articles is inserted between porous ceramic plate and porous metal plate so molded ratircles is not deformed. The temperature of hardening is 1000C ~ 2000CD, more desirable the temperature of hardening is 15O0C ~ 18O0C. The time of hardening is 10 ~ 100 minutes. So thermoset resin is dispersed uniformly in molded articles. The fuel cell electrical conductivity is 100 - 275 S/cm and elastic modulus is 40 ~ 55 MPa
[38] In case The electrical conductivity and elastic modulus is high efficiency and stability of fuel cell is improved. If the temperature of hardening is below 1000C the composite to be hardened non perfectively and If the temperature of hardening is higher 2000C the composite to be over hardened, and If the time of hardening is below 10 minutes the composite to be hardened non perfectively and If the time of hardening is higher than 100 minutes the composite to be over-hardened so conductivity is deteriorated. So temperature of hardening is at 1000C to 2000C and the time of hardening is at 10 minutes to 100 minutes.
[39] As described, the present invention is fuel cell separator and manufacturing method, described below comparative and example.
[40] Example 1
[41] ( The fuel cell separator manufacture composite mixed spheroidized graphite powder and phenol resin powder)
[42] At manufacturing of separator the composite is mixed 90 wt.% graphite power and
10 wt.% phenol resin powder in dry process and the composite to be tamped mold variably and formed in normal temperature at compressed pressure. In this time dry type mixer is super mixer, Hentschel mixer, weightlessness mixer.
[43] Exmaple2
[44] The separator manufactured as Example 1, At manufacturing of separator the composite is mixed 85 wt.% graphite power and 15 wt.% phenol resin powder in dry process
[45] Example3
[46] The separator manufactured as Example 1, At manufacturing of separator the composite is mixed 80 wt.% graphite power and 20 wt.% phenol resin powder in dry process
[47] Example4
[48] (The fuel cell separator manufacture composite mixed spheroidized graphite
powder and epoxy resin powder) [49] At manufacturing of separator the composite is mixed 90 wt.% graphite power and
9 wt.% epoxy resin powder and hardener 1 wt.% in dry process and the composite to be tamped mold variably and formed in normal temperature at compressed pressure. In this time dry type mixer is super mixer, Hentschel mixer, weightlessness mixer.
[50] Example5
[51] The separator manufactured as Example 4, At manufacturing of separator the composite is mixed 85 wt.% graphite power and 13.5 wt.% epoxy resin powder and hardener 1.5 wt.% [52] Exampleβ
[53] The separator manufactured as Example 4, At manufacturing of separator the composite is mixed 80 wt.% graphite power and 18 wt.% epoxy resin powder and hardener 2 wt.% [54] Example7
[55] At manufacturing of separator the composite is mixed 85.5 wt.% spheroidized graphite powder and 4.0 wt.% granulized carbon fiber and Ketjen Black 0.5 wt.% and
10 wt.% phenol resin powder in dry porcess and the composite to be tamped mold variably and formed in normal temperature at compressed pressure.
[56] Comparative 1
[57] (The fuel cell separator manufacture composite mixed needle graphite or plate graphite powder and resin powder in dry process) [58] At manufacturing of separator composite is mixed 90 wt.% graphite power of which mean diameter is 50 -100 μm of needle graphite or plate graphite and 10 wt.% phenol resin powder in dry process and the composite to be tamped mold variably and formed in normal temperature at compressed pressure. [59] Comparative 2
[60] (The fuel cell separator manufacture composite mixed in wet process)
[61] The total quantity of composit is 100 wt. % which ratio of composite is mixed 90 wt.% graphite power and 10 wt.% phenol resin powder in wet process and the quantity of solvent methyl ethyl ketone 150 wt.% and the composite to be mixed in 5O0C at 5hr and the composite is mixed in mixer and tamped mold variably and formed in normal temperature at compressed pressure. [62] Comparative 3
[63] Comparative 3 is the separator manufactured as Example 1, the separator is tamped mold uniformly and formed in normal temperature at compressed pressure [64] Comparative 4
[65] Comparative 4 is the separator manufactured as Example 4, the separator is tamped mold uniformly and formed in normal temperature at compressed pressure
[66] Table 1 is showing formability, electric conductivity and elastic modulus of
Example 4, 2, 3, 4, 5, 6 and 7 comparative 1 and 2. [67] [Table 1]
[68] Said formability is comparing of molded articles discharged from mold. That result is marking that good:o, not good:Δ, disapproval:x. The electrical conductivity is measured by 4 terminal measuring machine and elastic modulus is measured by ASTM
D790(thickness 2mm). [69] Table 2 is showing dispersion of thickness manufactured fuel cell separator by
Example 1, 4, Comparative 3 and 4.
Industrial Applicability [70] As described above, graphite composite fuel cell separator of the present invention is gaining time to shorten the time of forming to manufacture of graphite composite mixing spheroidized graphite powder and thermoset resin powder having similar apparent density. [71] The graphite composite fuel cell separator of the present invention have good electrical conductivity higher than 100 S/cm and good elastic modulus higher than 40
MPa [72] The graphite composite fuel cell separator of the present invention have efficiency and safety to have size precision of dispersion of separator thickness to below ± 30 μm to tamp variably along to path [73] The graphite composite fuel cell separator of the present invention is saving time to form because mold is possible to form not necessary to heat and to cool.
Claims
[1] A method of manufacturing graphite composite fuel cell separator, comprising the step of; manufacturing of composite mixing uniformly natural graphite power 70 wt.% ~ 95 wt.% and thermoset powder 5 wt.% ~ 30 wt.% in dry process; tamping variably to mold to be grooved said composite; forming compressively to 90-100% of theoretical density to be molded article; hardening by heat said molded article to remain in 10-100 minutes and 1000C - 2000C.
[2] The method of claim 1 wherein said natural graphite powder includes spheroidized graphite to fabricate mechanically needle graphite or layered sheet graphite having mean mesh of powder at 10 to 100 μm and spheroidized index at 0.5 to 1.0 and apparent density at 0.5 to 1.0 g/cm
[3] The method of claim 1 wherein said thermoset powder includes phenol resin implicating hardener or epoxy resin having mean mesh of powder at 10 to 150 μm and apparent density at 0.1 to 1.0 g/cm .
[4] The method of claim 1 wherein said manufacturing of composite mixing uniformly natural graphite power and thermoset powder in dry process includes additives such as carbon fiber or carbon black at 0.1 wt.% - 5.0 wt.%.
[5] The method of claim 1 wherein said manufacturing of composite mixing uniformly natural graphite power and thermoset powder in dry process using dry type mixer
[6] The method of claim 1 wherein said tamping variably to mold to be grooved said composite includes tamping grooved part and non grooved part in different tamping density to minimize of dispersion of thickness and to increase size precision in forming.
[7] The method of claim 1 or claim 6, wherein said tamping variably to mold to be grooved said composite includes tamping by gas tamping non-uniformly.
[8] The method of claim 1 or claim 6, wherein said tamping variably to mold to be grooved said composite includes tamping by multi-layer tamping.
[9] A fuel cell separator comprise the graphite composite including natural graphite powder and thermoset to have the smaller index than 30 μm at size precision index and have the more strength than 100 S/cm at bending strength.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| KR1020060064721A KR100781628B1 (en) | 2006-07-11 | 2006-07-11 | Fuel cell separator using the graphite composite and preparing method thereof |
| KR10-2006-0064721 | 2006-07-11 |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| WO2008007886A1 true WO2008007886A1 (en) | 2008-01-17 |
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Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| PCT/KR2007/003331 WO2008007886A1 (en) | 2006-07-11 | 2007-07-10 | Fuel cell separator using the graphite composite and preparing method thereof |
Country Status (2)
| Country | Link |
|---|---|
| KR (1) | KR100781628B1 (en) |
| WO (1) | WO2008007886A1 (en) |
Families Citing this family (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR100977765B1 (en) * | 2007-12-21 | 2010-08-24 | 재단법인 포항산업과학연구원 | Fabrication method of a carbonaceous bipolar plate for PEMFC |
| KR101197288B1 (en) | 2012-02-13 | 2012-11-05 | 금호석유화학 주식회사 | Carbon nano-material pellets and a method for preparing the pellets from powder of carbon nano-material |
| US10629916B2 (en) | 2014-09-01 | 2020-04-21 | Korea Institute Of Industrial Technology | Preparation method for bipolar plate for redox flow battery |
| KR20220031376A (en) | 2020-09-04 | 2022-03-11 | 파셀 주식회사 | A Fuel cell stack comprising bipolar plate having embossed structure |
Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001126744A (en) * | 1999-10-28 | 2001-05-11 | Osaka Gas Co Ltd | Separator for fuel cell and fabricating method therefor |
| KR20020053883A (en) * | 1999-11-26 | 2002-07-05 | 팀칼 아게 | Method for producing graphite powder with an increased bulk density |
| US20030027030A1 (en) * | 2001-07-26 | 2003-02-06 | Matsushita Electric Industrial Co., Ltd. | Fuel-cell separator, production of the same, and fuel cell |
| JP2003109622A (en) * | 2001-07-26 | 2003-04-11 | Matsushita Electric Ind Co Ltd | Fuel cell separator, method of manufacturing the same, and fuel cell |
Family Cites Families (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4269642A (en) | 1979-10-29 | 1981-05-26 | United Technologies Corporation | Method of forming densified edge seals for fuel cell components |
| JPS62270412A (en) | 1986-05-16 | 1987-11-24 | Kawasaki Steel Corp | Production of carbon board |
| KR20050120515A (en) * | 2004-06-19 | 2005-12-22 | 한국타이어 주식회사 | A carbon composite, method for preparing the same, a fuel cell separator using the carbon composites |
| KR20050090457A (en) * | 2005-07-14 | 2005-09-13 | 에이키 쯔시마 | Method for producing separator of fuel cell |
-
2006
- 2006-07-11 KR KR1020060064721A patent/KR100781628B1/en not_active IP Right Cessation
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2007
- 2007-07-10 WO PCT/KR2007/003331 patent/WO2008007886A1/en active Application Filing
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001126744A (en) * | 1999-10-28 | 2001-05-11 | Osaka Gas Co Ltd | Separator for fuel cell and fabricating method therefor |
| KR20020053883A (en) * | 1999-11-26 | 2002-07-05 | 팀칼 아게 | Method for producing graphite powder with an increased bulk density |
| US20030027030A1 (en) * | 2001-07-26 | 2003-02-06 | Matsushita Electric Industrial Co., Ltd. | Fuel-cell separator, production of the same, and fuel cell |
| JP2003109622A (en) * | 2001-07-26 | 2003-04-11 | Matsushita Electric Ind Co Ltd | Fuel cell separator, method of manufacturing the same, and fuel cell |
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| Publication number | Publication date |
|---|---|
| KR100781628B1 (en) | 2007-12-03 |
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