WO2023121132A1 - 연료전지 분리판용 스테인리스강 및 그 제조 방법 - Google Patents
연료전지 분리판용 스테인리스강 및 그 제조 방법 Download PDFInfo
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- WO2023121132A1 WO2023121132A1 PCT/KR2022/020356 KR2022020356W WO2023121132A1 WO 2023121132 A1 WO2023121132 A1 WO 2023121132A1 KR 2022020356 W KR2022020356 W KR 2022020356W WO 2023121132 A1 WO2023121132 A1 WO 2023121132A1
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- Prior art keywords
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- fuel cell
- stainless steel
- metal material
- cell separator
- Prior art date
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- 239000000446 fuel Substances 0.000 title claims abstract description 31
- 229910001220 stainless steel Inorganic materials 0.000 title claims description 28
- 239000010935 stainless steel Substances 0.000 title description 19
- 238000004519 manufacturing process Methods 0.000 title description 6
- 239000007769 metal material Substances 0.000 claims abstract description 25
- 238000000034 method Methods 0.000 claims description 14
- 229910052799 carbon Inorganic materials 0.000 claims description 9
- 229910052757 nitrogen Inorganic materials 0.000 claims description 9
- 229910000963 austenitic stainless steel Inorganic materials 0.000 claims description 8
- 239000012535 impurity Substances 0.000 claims description 8
- 229910052758 niobium Inorganic materials 0.000 claims description 7
- 229910052720 vanadium Inorganic materials 0.000 claims description 7
- 229910052748 manganese Inorganic materials 0.000 claims description 6
- 229910052719 titanium Inorganic materials 0.000 claims description 6
- 229910052802 copper Inorganic materials 0.000 claims description 3
- 229910052750 molybdenum Inorganic materials 0.000 claims description 3
- 229910052759 nickel Inorganic materials 0.000 claims description 3
- 230000005540 biological transmission Effects 0.000 abstract description 7
- 230000007797 corrosion Effects 0.000 description 13
- 238000005260 corrosion Methods 0.000 description 13
- 230000000052 comparative effect Effects 0.000 description 12
- 239000011651 chromium Substances 0.000 description 11
- 229910000831 Steel Inorganic materials 0.000 description 10
- 239000010959 steel Substances 0.000 description 10
- 239000002253 acid Substances 0.000 description 9
- 229910001566 austenite Inorganic materials 0.000 description 8
- 239000000463 material Substances 0.000 description 7
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 description 6
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 4
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 4
- 230000015572 biosynthetic process Effects 0.000 description 4
- 230000007423 decrease Effects 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 238000005097 cold rolling Methods 0.000 description 3
- 238000005098 hot rolling Methods 0.000 description 3
- 238000007654 immersion Methods 0.000 description 3
- 239000000203 mixture Substances 0.000 description 3
- 238000005096 rolling process Methods 0.000 description 3
- 230000000087 stabilizing effect Effects 0.000 description 3
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 2
- 238000000137 annealing Methods 0.000 description 2
- UFGZSIPAQKLCGR-UHFFFAOYSA-N chromium carbide Chemical compound [Cr]#C[Cr]C#[Cr] UFGZSIPAQKLCGR-UHFFFAOYSA-N 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 238000009792 diffusion process Methods 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 229910017604 nitric acid Inorganic materials 0.000 description 2
- 238000002161 passivation Methods 0.000 description 2
- 238000005498 polishing Methods 0.000 description 2
- 229910003470 tongbaite Inorganic materials 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 239000010960 cold rolled steel Substances 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 238000010297 mechanical methods and process Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 238000005728 strengthening Methods 0.000 description 1
- 238000005211 surface analysis Methods 0.000 description 1
- 230000003746 surface roughness Effects 0.000 description 1
- 229910000859 α-Fe Inorganic materials 0.000 description 1
Images
Classifications
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- 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
- H01M8/0206—Metals or alloys
- H01M8/0208—Alloys
- H01M8/021—Alloys based on iron
-
- 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
Definitions
- the present invention relates to stainless steel for polymer fuel cell separators having low contact resistance and a method for manufacturing the same, and more particularly, to secure low contact resistance by increasing the contact area with GDL (Gas Diffusion Layer) by controlling the shape of the surface of the separator. It relates to a stainless steel for a fuel cell separator capable of.
- GDL Gas Diffusion Layer
- a fuel cell stack is in the form of stacking cells composed of a Membrane Electrode Assembly (MEA) including electrolyte, electrodes, and GDL, and a separator. Therefore, the bipolar plate is in contact with the GDL, and the performance of the cell and the fuel cell is reduced due to contact resistance, which is a resistance generated at the bipolar plate/GDL interface.
- MEA Membrane Electrode Assembly
- the contact resistance of such a separator is mainly influenced by two things.
- the first is a passivation film, which is an oxide layer on the surface of a metal separator. Passive film is a method to secure high corrosion resistance, but in terms of contact resistance, it is good to have a thin thickness as possible because it is a non-conductive oxide layer.
- the second thing that affects the contact resistance is the contact area between the separator and the GDL. Since the separator and GDL are objects with different surface roughness, the actual contact area between the two objects in contact has a great effect on the contact resistance. If the contact area between the separator and the GDL is large, the contact resistance tends to be low, and if the contact area is small, the contact resistance tends to be high, so the contact resistance reduction effect varies depending on how the surface shape of the separator is changed.
- the thickness of the separator material is a lot of thin ultra-thin materials of the order of tens to hundreds of ⁇ m, and the ultra-thin materials are subjected to bright annealing in the manufacturing process. Therefore, it has a bright annealed surface with almost no surface curvature, and if such a material is used as a separator plate, there is a problem in that the contact area with GDL is small and the contact resistance is increased. Therefore, in order to reduce the contact resistance, it is necessary to increase the contact area with the GDL by making the shape of the surface of the separator rugged.
- an object of the present invention is to provide stainless steel having low contact resistance by forming fine protrusions on the surface as a material for a fuel cell separator.
- the number of fine protrusions between 10 and 100 nm is 5 or more on the surface of the metal material in contact with the GDL in the fuel cell, and observed with a transmission electron microscope (TEM).
- TEM transmission electron microscope
- the ratio of real surface length/apparent surface length without protrusions is 1.15 or more based on one cross section.
- the metal material contains, by weight, Cr: 15 to 35%, C: 0.02% or less, N: 0.02% or less, Si: 0.4% or less, S: 0.003% or less, Mn: 0.2% or less, Cu: 2% or less, the balance may be a ferritic stainless steel containing Fe and other unavoidable impurities.
- the metal material contains, by weight, Cr: 15 to 30%, Ni: 7 to 15%, C: 0.09% or less, Si: 2.5% or less. , S: 0.003% or less, Mn: 3% or less, Mo: 3% or less, N: 0.3% or less, the balance may be an austenitic stainless steel containing Fe and other unavoidable impurities.
- a separator having low contact resistance can be manufactured without an expensive coating process in a fuel cell environment.
- FIG. 1 is a cross-section of a fuel cell bipolar plate observed with a transmission electron microscope according to the present invention, in which five or more fine protrusions having a height of 10 to 100 nm or less are present and the actual surface length is 15% or more longer than the apparent surface length without protrusions. .
- FIG. 2 is a cross-section of a fuel cell bipolar plate without protrusions observed through a transmission electron microscope.
- the number of fine protrusions between 10 and 100 nm is 5 or more on the surface of the metal material in contact with the GDL in the fuel cell, and observed with a transmission electron microscope (TEM).
- TEM transmission electron microscope
- the ratio of real surface length/apparent surface length without protrusions is 1.15 or more based on one cross section.
- the number of fine protrusions between 10 and 100 nm is 5 or more on the surface of the metal material in contact with the GDL in the fuel cell, and observed with a transmission electron microscope (TEM).
- TEM transmission electron microscope
- the ratio of real surface length/apparent surface length without protrusions is 1.15 or more based on one cross section.
- the actual surface area is increased compared to the apparent surface area, thereby increasing the contact area with GDL and reducing contact resistance. If the height of the protrusion is too low, less than 10 nm, the effect on the increase in surface area due to the protrusion is insignificant, and if the height of the protrusion is too high, exceeding 100 nm, the number of protrusions per unit area decreases, so the effect on the increase in surface area is reduced.
- the separator according to the embodiment of the present invention is characterized in that the contact resistance value is 10 m ⁇ cm 2 or less.
- the metal material contains, by weight, Cr: 15 to 35%, C: 0.02% or less, N: 0.02% or less, Si: 0.4% or less, S: 0.003% or less, Mn: 0.2% or less, Cu: 2% or less, the balance may be a ferritic stainless steel containing Fe and other unavoidable impurities.
- the metal material for the fuel cell separator is that the ferritic stainless steel further contains at least one selected from the group consisting of Ti, Nb, and V in a total amount of 1.0% or less.
- an element that stabilizes the austenite phase As an element that replaces the Ni element, it has the advantage of improving strength and pitting resistance, but has the disadvantage of lowering workability such as elongation, so in the present invention, it is limited to 0.02% or less.
- minor impurity element it is the main element that segregates at grain boundaries and causes working cracks during hot rolling, so it is limited to 0.003% or less, which is the lowest possible content.
- austenite phase stabilizing element as an element that replaces Ni, when added in ferrite steel by metastabilizing the austenite phase, strength is increased and workability is reduced, so the content is limited to 0.2% or less.
- the metal material for a fuel cell separator according to an embodiment of the present invention, contains, by weight, Cr: 15-30%, Ni: 7-15%, C: 0.09% or less, Si: 2.5% or less, S : 0.003% or less, Mn: 3% or less, Mo: 3% or less, N: 0.3% or less, the balance may be an austenitic stainless steel containing Fe and other unavoidable impurities.
- the metal material for the fuel cell separator further includes at least one or more selected from the group consisting of Ti, Nb, and V in the austenitic stainless steel at a total amount of 1.0% or less. can do.
- minor impurity element it is the main element that segregates at grain boundaries and causes working cracks during hot rolling, so it is limited to 0.003% or less, which is the lowest possible content.
- Ni is an element that replaces Ni as an austenite phase stabilizing element, but it is limited to 3.0% or less because corrosion resistance deteriorates when excessively added.
- a method for controlling the surface shape of stainless steel may be manufactured through the following process.
- the surface shape of stainless steel can be controlled chemically or mechanically.
- the surface shape can be controlled by immersing stainless steel in an acid solution.
- the acid solution for immersing stainless steel may be hydrochloric acid or sulfuric acid or nitric acid or hydrofluoric acid, and two or more acid solutions may be mixed and used, or two or more acid solutions may be sequentially immersed.
- the surface shape of stainless steel can be controlled by performing electrolytic treatment, and may include electrolytic treatment before and after immersion in an acid solution.
- the surface shape may vary depending on the type, temperature, concentration, etc. of the acid solution, the immersion time, and the applied current of the electrolytic treatment.
- a surface shape having excellent contact resistance can be obtained by immersing for a time of 30 seconds to 300 seconds using 5 to 20% hydrochloric acid or 5% to 20% hydrofluoric acid as an acid solution.
- the surface shape of stainless steel can be controlled through mechanical polishing rather than the chemical method, and the surface shape can be changed by the type, thickness, shape, and distribution of the abrasive during polishing.
- the surface shape according to the present application is not limited to the above-described chemical or mechanical methods, and may be derived by various conditions and methods.
- Table 1 shows alloy components of all examples including comparative examples and inventive examples of ferritic and austenitic stainless steels.
- the stainless steel used in the present invention after preparing a cold-rolled sheet using a Z-mill cold rolling mill from stainless steel having the above composition in the cold-rolling step, bright annealing was performed on the cold-rolled sheet in the heat treatment step.
- Steel A is a ferritic stainless steel according to the present invention
- steel B relates to an austenitic stainless steel according to the present invention.
- surface shapes of ferritic and austenitic stainless steels are controlled.
- the relationship between the contact resistance and the surface shape index was investigated, which is shown in Table 2 below.
- Table 2 is a table showing the surface analysis results and contact resistance measurement values of the manufactured cold-rolled steel sheets, and the average height of protrusions, the number of protrusions between 10 and 100 nm, and the actual surface length/apparent surface length are determined by examining the cross section of the steel sheet with a transmission electron microscope. (TEM) was used. Surface protrusions effective for contact resistance are fine protrusions with a height of several tens of nm, so it is difficult to observe with a low-magnification scanning electron microscope (SEM). After observing 10 places for each specimen, the average was taken.
- SEM scanning electron microscope
- interfacial contact resistance For the evaluation of interfacial contact resistance in Table 2, after preparing two sheets of the manufactured material, carbon paper (SGL-10BA) used as a gas diffusion layer was placed between them. The interfacial contact resistance at a contact pressure of 100 N/cm 2 was evaluated 5 times, and then averaged.
- Examples 1 to 7 having fine protrusions on the surface defined by the present invention had excellent contact resistance of 10 m ⁇ cm 2 or less. Although the average protrusion height did not have a significant correlation with the contact resistance, the contact resistance tended to decrease as the number of fine protrusions between 10 and 100 nm increased. In addition, as the number of fine protrusions between 10 and 100 nm on the surface increased, the actual surface length tended to increase compared to the apparent surface length. Through this, it is thought that the actual contact area with the GDL as a separator increased and the contact resistance decreased.
- Comparative Examples 1 to 9 were surfaces with no or very small number of fine protrusions between 10 and 100 nm, which are limited by the present invention, and their contact resistance exceeded 10 m ⁇ cm 2 .
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- Life Sciences & Earth Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Fuel Cell (AREA)
Abstract
Description
강종 | C | Si | S | Mn | Cr | Mo | Ni, Nb, V, Ti | N | Cu |
A강 | 0.008 | 0.1 | 0.0005 | 0.1 | 30 | - | Nb: 0.2V: 0.4 Ti: 0.1 |
0.015 | 0.06 |
B강 | 0.020 | 2.0 | 0.0009 | 0.7 | 23 | 0.2 | Ni: 12 | 0.200 | - |
실험 No. | 강종 | 돌기 평균 높이 (㎛) | 10~100nm 사이의 돌기 개수(개/㎛) | 실제 표면길이/겉보기 표면길이 | 접촉저항(mΩ·cm 2 ) |
비교예1 | A강 | 0.26 | 0 | 1.00 | 51.2 |
비교예2 | A강 | 0.19 | 0 | 1.02 | 33.9 |
비교예3 | A강 | 0.18 | 0 | 1.02 | 29.0 |
비교예4 | B강 | 0.28 | 0 | 1.01 | 102.6 |
비교예5 | B강 | 0.20 | 0 | 1.01 | 34.2 |
비교예6 | B강 | 0.18 | 0 | 1.01 | 25.1 |
비교예7 | B강 | 0.16 | 1 | 1.02 | 12.4 |
비교예8 | A강 | 0.15 | 1 | 1.04 | 14.5 |
비교예9 | A강 | 0.14 | 1 | 1.05 | 12.5 |
실시예1 | B강 | 0.15 | 5 | 1.15 | 9.6 |
실시예2 | A강 | 0.13 | 9 | 1.18 | 8.1 |
실시예3 | B강 | 0.14 | 11 | 1.19 | 7.9 |
실시예4 | A강 | 0.13 | 11 | 1.22 | 6.3 |
실시예5 | B강 | 0.13 | 12 | 1.27 | 6.6 |
실시예6 | B강 | 0.14 | 13 | 1.31 | 6.0 |
실시예7 | A강 | 0.14 | 16 | 1.36 | 5.7 |
Claims (5)
- 연료전지 내 GDL과 접촉하는 금속재료 표면이 10~100nm 사이의 미세 돌기의 개수가 5개 이상이면서, 투과전자현미경(TEM)으로 관찰한 단면을 기준으로 실제 표면길이(real surface length)/돌기가 없는 겉보기 표면길이 (apparent surface length)의 비가 1.15 이상인 연료전지 분리판용 금속재료.
- 청구항 1에 있어서,상기 금속재료가 중량%로 Cr: 15~35%, C: 0.02% 이하, N: 0.02% 이하, Si: 0.4% 이하, S: 0.003% 이하, Mn: 0.2% 이하, Cu: 2% 이하, 잔부 Fe 및 기타 불가피한 불순물을 포함하는 페라이트계 스테인리스강인 연료전지 분리판용 금속재료.
- 청구항 2에 있어서,상기 페라이트계 스테인리스강이 Ti, Nb, 및 V로 이루어지는 군에서 선택되는 적어도 1종 이상을 합계로 1.0% 이하로 더 포함하는 연료전지 분리판용 금속재료.
- 청구항 1에 있어서,상기 금속재료가 중량%로 Cr: 15~30%, Ni: 7~15%, C: 0.09% 이하, Si: 2.5% 이하, S: 0.003% 이하, Mn: 3% 이하, Mo: 3% 이하, N: 0.3% 이하, 잔부 Fe 및 기타 불가피한 불순물을 포함하는 오스테나이트계 스테인리스강인 연료전지 분리판용 금속재료.
- 청구항 4에 있어서상기 오스테나이트계 스테인리스강이 Ti, Nb, 및 V로 이루어지는 군에서 선택되는 적어도 1종 이상을 합계로 1.0% 이하로 더 포함하는 연료전지 분리판용 금속재료.
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CN202280084042.0A CN118355531A (zh) | 2021-12-20 | 2022-12-14 | 燃料电池隔板用不锈钢及其制造方法 |
CA3240299A CA3240299A1 (en) | 2021-12-20 | 2022-12-14 | Stainless steel for fuel cell separator and manufacturing method thereof |
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KR1020210183089A KR20230093983A (ko) | 2021-12-20 | 2021-12-20 | 연료전지 분리판용 스테인리스강 및 그 제조 방법 |
KR10-2021-0183089 | 2021-12-20 |
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KR20140039326A (ko) * | 2011-07-29 | 2014-04-01 | 제이에프이 스틸 가부시키가이샤 | 연료 전지 세퍼레이터용 스테인리스강 |
WO2018043285A1 (ja) * | 2016-08-30 | 2018-03-08 | 新日鐵住金株式会社 | フェライト系ステンレス鋼材、セパレーター、セルおよび燃料電池 |
WO2019058409A1 (ja) * | 2017-09-19 | 2019-03-28 | 新日鐵住金株式会社 | ステンレス鋼板及びその製造方法、固体高分子型燃料電池用セパレータ、固体高分子型燃料電池セル、並びに固体高分子型燃料電池 |
KR20210100762A (ko) * | 2017-04-25 | 2021-08-17 | 제이에프이 스틸 가부시키가이샤 | 연료 전지의 세퍼레이터용의 스테인리스 강판 및 그 제조 방법 |
KR20210147646A (ko) * | 2020-05-29 | 2021-12-07 | 주식회사 포스코 | 연료전지 분리판용 스테인리스강 |
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2021
- 2021-12-20 KR KR1020210183089A patent/KR20230093983A/ko unknown
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2022
- 2022-12-14 CN CN202280084042.0A patent/CN118355531A/zh active Pending
- 2022-12-14 CA CA3240299A patent/CA3240299A1/en active Pending
- 2022-12-14 WO PCT/KR2022/020356 patent/WO2023121132A1/ko active Application Filing
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KR20140039326A (ko) * | 2011-07-29 | 2014-04-01 | 제이에프이 스틸 가부시키가이샤 | 연료 전지 세퍼레이터용 스테인리스강 |
WO2018043285A1 (ja) * | 2016-08-30 | 2018-03-08 | 新日鐵住金株式会社 | フェライト系ステンレス鋼材、セパレーター、セルおよび燃料電池 |
KR20210100762A (ko) * | 2017-04-25 | 2021-08-17 | 제이에프이 스틸 가부시키가이샤 | 연료 전지의 세퍼레이터용의 스테인리스 강판 및 그 제조 방법 |
WO2019058409A1 (ja) * | 2017-09-19 | 2019-03-28 | 新日鐵住金株式会社 | ステンレス鋼板及びその製造方法、固体高分子型燃料電池用セパレータ、固体高分子型燃料電池セル、並びに固体高分子型燃料電池 |
KR20210147646A (ko) * | 2020-05-29 | 2021-12-07 | 주식회사 포스코 | 연료전지 분리판용 스테인리스강 |
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