EP3900089A1 - Fuel cell or electrolyser - Google Patents
Fuel cell or electrolyserInfo
- Publication number
- EP3900089A1 EP3900089A1 EP19835608.1A EP19835608A EP3900089A1 EP 3900089 A1 EP3900089 A1 EP 3900089A1 EP 19835608 A EP19835608 A EP 19835608A EP 3900089 A1 EP3900089 A1 EP 3900089A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- fuel cell
- metal
- metal oxide
- electrolyzer according
- carrier
- Prior art date
- Legal status (The legal status 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 status listed.)
- Pending
Links
- 239000000446 fuel Substances 0.000 title claims abstract description 38
- 239000003054 catalyst Substances 0.000 claims abstract description 67
- 229910044991 metal oxide Inorganic materials 0.000 claims abstract description 59
- 150000004706 metal oxides Chemical class 0.000 claims abstract description 59
- 239000000463 material Substances 0.000 claims abstract description 30
- 229910001463 metal phosphate Inorganic materials 0.000 claims abstract description 30
- 229910052751 metal Inorganic materials 0.000 claims abstract description 22
- 239000002184 metal Substances 0.000 claims abstract description 22
- 239000012528 membrane Substances 0.000 claims abstract description 12
- 239000005518 polymer electrolyte Substances 0.000 claims abstract description 12
- 125000005341 metaphosphate group Chemical class 0.000 claims abstract description 5
- 239000000126 substance Substances 0.000 claims abstract description 5
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 44
- 229910052697 platinum Inorganic materials 0.000 claims description 22
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 18
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 18
- 239000001301 oxygen Substances 0.000 claims description 18
- 229910052760 oxygen Inorganic materials 0.000 claims description 18
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 claims description 9
- 229910052741 iridium Inorganic materials 0.000 claims description 9
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 claims description 9
- 229910052757 nitrogen Inorganic materials 0.000 claims description 9
- 229910052707 ruthenium Inorganic materials 0.000 claims description 9
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims description 9
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 8
- 229910052799 carbon Inorganic materials 0.000 claims description 8
- 229910052731 fluorine Inorganic materials 0.000 claims description 8
- 239000011737 fluorine Substances 0.000 claims description 8
- 229910052715 tantalum Inorganic materials 0.000 claims description 8
- 229910052758 niobium Inorganic materials 0.000 claims description 7
- 239000010955 niobium Substances 0.000 claims description 7
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims description 7
- 239000001257 hydrogen Substances 0.000 claims description 6
- 229910052739 hydrogen Inorganic materials 0.000 claims description 6
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 4
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 4
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims description 4
- 239000013078 crystal Substances 0.000 claims description 4
- 229910052735 hafnium Inorganic materials 0.000 claims description 4
- VBJZVLUMGGDVMO-UHFFFAOYSA-N hafnium atom Chemical compound [Hf] VBJZVLUMGGDVMO-UHFFFAOYSA-N 0.000 claims description 4
- 230000002209 hydrophobic effect Effects 0.000 claims description 4
- 229920000554 ionomer Polymers 0.000 claims description 4
- 229910052719 titanium Inorganic materials 0.000 claims description 4
- 239000010936 titanium Substances 0.000 claims description 4
- 229910052726 zirconium Inorganic materials 0.000 claims description 4
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 claims description 3
- 229910052718 tin Inorganic materials 0.000 claims description 3
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 claims description 2
- 229910052782 aluminium Inorganic materials 0.000 claims description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 2
- 229910052796 boron Inorganic materials 0.000 claims description 2
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 claims 2
- 239000000758 substrate Substances 0.000 abstract description 2
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 19
- 230000000694 effects Effects 0.000 description 16
- BPUBBGLMJRNUCC-UHFFFAOYSA-N oxygen(2-);tantalum(5+) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ta+5].[Ta+5] BPUBBGLMJRNUCC-UHFFFAOYSA-N 0.000 description 10
- 229910001936 tantalum oxide Inorganic materials 0.000 description 10
- OPBPKFFRPGKDIG-UHFFFAOYSA-A tantalum(5+) pentaphosphate Chemical class [Ta+5].[Ta+5].[Ta+5].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O OPBPKFFRPGKDIG-UHFFFAOYSA-A 0.000 description 10
- 229910001887 tin oxide Inorganic materials 0.000 description 10
- 230000009467 reduction Effects 0.000 description 9
- 239000007789 gas Substances 0.000 description 8
- 239000002245 particle Substances 0.000 description 8
- 239000012071 phase Substances 0.000 description 7
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 description 6
- 238000006243 chemical reaction Methods 0.000 description 6
- 230000007062 hydrolysis Effects 0.000 description 6
- 238000006460 hydrolysis reaction Methods 0.000 description 6
- 238000010587 phase diagram Methods 0.000 description 6
- 239000011248 coating agent Substances 0.000 description 5
- 238000000576 coating method Methods 0.000 description 5
- 238000009792 diffusion process Methods 0.000 description 5
- 238000000034 method Methods 0.000 description 5
- 239000000843 powder Substances 0.000 description 5
- 230000008569 process Effects 0.000 description 5
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 4
- 229920000557 Nafion® Polymers 0.000 description 4
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 4
- 229910019142 PO4 Inorganic materials 0.000 description 4
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 4
- 229910000484 niobium oxide Inorganic materials 0.000 description 4
- URLJKFSTXLNXLG-UHFFFAOYSA-N niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Nb+5].[Nb+5] URLJKFSTXLNXLG-UHFFFAOYSA-N 0.000 description 4
- 229920000388 Polyphosphate Polymers 0.000 description 3
- 125000004429 atom Chemical group 0.000 description 3
- 230000007774 longterm Effects 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 239000000203 mixture Substances 0.000 description 3
- 235000021317 phosphate Nutrition 0.000 description 3
- 239000001205 polyphosphate Substances 0.000 description 3
- 235000011176 polyphosphates Nutrition 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- 238000004544 sputter deposition Methods 0.000 description 3
- 229910000166 zirconium phosphate Inorganic materials 0.000 description 3
- LEHFSLREWWMLPU-UHFFFAOYSA-B zirconium(4+);tetraphosphate Chemical compound [Zr+4].[Zr+4].[Zr+4].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O LEHFSLREWWMLPU-UHFFFAOYSA-B 0.000 description 3
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 2
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 2
- 230000002378 acidificating effect Effects 0.000 description 2
- LFVGISIMTYGQHF-UHFFFAOYSA-N ammonium dihydrogen phosphate Chemical compound [NH4+].OP(O)([O-])=O LFVGISIMTYGQHF-UHFFFAOYSA-N 0.000 description 2
- 229910000387 ammonium dihydrogen phosphate Inorganic materials 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 238000006555 catalytic reaction Methods 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 229910017052 cobalt Inorganic materials 0.000 description 2
- 239000010941 cobalt Substances 0.000 description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 2
- 239000002131 composite material Substances 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 239000004020 conductor Substances 0.000 description 2
- 230000002349 favourable effect Effects 0.000 description 2
- 229910052742 iron Inorganic materials 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 229910052750 molybdenum Inorganic materials 0.000 description 2
- 239000011733 molybdenum Substances 0.000 description 2
- 235000019837 monoammonium phosphate Nutrition 0.000 description 2
- 229910052759 nickel Inorganic materials 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- 239000000615 nonconductor Substances 0.000 description 2
- 229910052763 palladium Inorganic materials 0.000 description 2
- 150000003013 phosphoric acid derivatives Chemical class 0.000 description 2
- 239000010970 precious metal Substances 0.000 description 2
- 239000000047 product Substances 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 230000035945 sensitivity Effects 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 2
- 229910052721 tungsten Inorganic materials 0.000 description 2
- 239000010937 tungsten Substances 0.000 description 2
- 229910052720 vanadium Inorganic materials 0.000 description 2
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 238000009736 wetting Methods 0.000 description 2
- ZGMMMTSCLMMPDI-UHFFFAOYSA-J 2,3-dihydroxybutanedioate;zirconium(4+) Chemical compound [Zr+4].[O-]C(=O)C(O)C(O)C([O-])=O.[O-]C(=O)C(O)C(O)C([O-])=O ZGMMMTSCLMMPDI-UHFFFAOYSA-J 0.000 description 1
- 229920001817 Agar Polymers 0.000 description 1
- FEWJPZIEWOKRBE-JCYAYHJZSA-N Dextrotartaric acid Chemical compound OC(=O)[C@H](O)[C@@H](O)C(O)=O FEWJPZIEWOKRBE-JCYAYHJZSA-N 0.000 description 1
- 241000206672 Gelidium Species 0.000 description 1
- 238000004566 IR spectroscopy Methods 0.000 description 1
- 229910001260 Pt alloy Inorganic materials 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000012072 active phase Substances 0.000 description 1
- 239000003463 adsorbent Substances 0.000 description 1
- 235000010419 agar Nutrition 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000005271 boronizing Methods 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- 238000010000 carbonizing Methods 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 150000001768 cations Chemical class 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
- 230000001427 coherent effect Effects 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 230000003203 everyday effect Effects 0.000 description 1
- 238000003682 fluorination reaction Methods 0.000 description 1
- 150000002222 fluorine compounds Chemical class 0.000 description 1
- 230000004927 fusion Effects 0.000 description 1
- 229910021397 glassy carbon Inorganic materials 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 238000002386 leaching Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 239000002105 nanoparticle Substances 0.000 description 1
- CNHRNMLCYGFITG-UHFFFAOYSA-A niobium(5+);pentaphosphate Chemical compound [Nb+5].[Nb+5].[Nb+5].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O CNHRNMLCYGFITG-UHFFFAOYSA-A 0.000 description 1
- 238000005121 nitriding Methods 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 238000012797 qualification Methods 0.000 description 1
- 230000007115 recruitment Effects 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 239000006104 solid solution Substances 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 229940095064 tartrate Drugs 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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
- H01M4/9025—Oxides specially used in fuel cell operating at high temperature, e.g. SOFC
- H01M4/9033—Complex oxides, optionally doped, of the type M1MeO3, M1 being an alkaline earth metal or a rare earth, Me being a metal, e.g. perovskites
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
- C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
- C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/92—Metals of platinum group
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/92—Metals of platinum group
- H01M4/925—Metals of platinum group supported on carriers, e.g. powder carriers
- H01M4/926—Metals of platinum group supported on carriers, e.g. powder carriers on carbon or graphite
-
- 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
- H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
- H01M8/1213—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the electrode/electrolyte combination or the supporting material
-
- B01J35/33—
-
- 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
Definitions
- the invention relates to a fuel cell or an electrolyser comprising at least one electrode and at least one polymer electrolyte membrane, the electrode comprising a catalyst system comprising a carrier metal oxide and a catalyst material.
- Catalyst systems of the type mentioned are for example from the
- Metal oxides are used as carriers for active catalyst substances comprising at least one noble metal.
- the use of such a catalyst system for forming an electrode unit and its use for a fuel cell or an electrolyzer is also described.
- the disadvantage of the catalyst system is the high proportion of precious metal that is required and thus increases the costs.
- the object is achieved for the fuel cell or the electrolyzer comprising at least one electrode and at least one polymer electrolyte membrane, the electrode comprising a catalyst system comprising a carrier metal oxide and a catalyst material, in that the catalyst material is formed by an electrically conductive metal phosphate, which is called metaphosphate of the general chemical formula Me z n + 2 (Pn03n + i) z, where
- n is in the range from 1 to 10.
- the catalyst system has the decisive advantage that large quantities of expensive precious metals can be avoided. This enables inexpensive, large-scale use of the catalyst system. It also has an extensive high electrical conductivity, good long-term stability and reduced sensitivity to hydrolysis.
- the electrically conductive metal phosphate has an electrical conductivity of at least 10 S / cm. This is achieved, for example, by doping the metal phosphate with doping elements.
- the phosphates can condense to ring-shaped metaphosphates and / or long-chain polyphosphates.
- PO4 -, P2O7 - and possible P3O10-5 - groups in the different niobium and tanphosphates were identified by infrared spectroscopy in some niobium and tantalum phosphates prepared from aqueous solution and then tempered. If the phosphates are prepared for the respective application area, it must be taken into account that the manufacturing conditions may differ from the operating conditions.
- the molecules which are usually tempered and condensed at higher temperatures, can hydrolyze to smaller units of the formula M z n +2 (Pn03n + i) z under the circumstances of use.
- a small amount of oxygen can also be incorporated, so that a small proportion of TaOPC can be formed and contained in, for example, tantalum phosphates.
- the degree of resistance to hydrolysis of the catalyst material is not least determined by the type of salt used, its solubility product, the free partial formation energies and the valency of the salt-forming cation.
- the following reactions with tantalum phosphate as catalyst material are formally conceivable:
- tantalum phosphate which can be produced from a tantalum trate complex and ammonium dihydrogen phosphate by a precipitation reaction and subsequent calcination at approx. 550 ° C, has proven to be extremely stable to hydrolysis.
- the metal phosphate is therefore particularly mesoporous.
- Polyphosphates such as tantalum polyphosphates, are strongly acidic and provide the protons in the catalytic reaction.
- the "acid-catalyzed" reaction via a proton donor is used for the invention, as suggested by the chemical reaction equation for oxygen reduction.
- a ratio of catalyst system to carrier metal oxide is particularly preferably 1:10.
- the carrier metal oxide preferably contains at least one metal from the group comprising: tin, tantalum, niobium, titanium, zirconium, hafnium, aluminum.
- the carrier metal oxide is further modified by doping with foreign atoms in such a way that the primary step of oxygen adsorption is facilitated. It has proven useful if the catalyst system continues to include platinum.
- the carrier metal oxide has, in particular, oxide grains which have a grain size in the range of> 50 nm.
- the electrically conductive metal phosphate preferably contains at least one metal from the group comprising: tantalum, niobium, titanium, zirconium, hafnium.
- the particularly favorable properties of these metals are based on the one hand in their high acidity and on the other hand in the very low solubility products in water. The latter property results in good long-term stability.
- Metal phosphates are preferably used on the carrier metal oxide, in particular made of electrically conductive metal oxide and / or modified metal oxide composites which comprise the same metal as the carrier metal oxide. For example, combinations of tantalum phosphate and tantalum oxide / tin oxide or of niobium phosphate and niobium oxide / tin oxide, etc. have proven particularly useful.
- the metal phosphate preferably has a grain size in the range ⁇ 50 nm. The nanoscale design of the metal phosphate creates high densities of lattice disorder, which significantly increase the electrical conductivity of the metal phosphate.
- the carrier metal oxide and / or the metal phosphate is doped with iridium and / or ruthenium.
- the carrier metal oxide has a first crystal lattice structure comprising first oxygen lattice sites and first metal lattice sites, the carrier metal oxide on the first oxygen lattice sites being doped with at least one element from the group comprising: fluorine, nitrogen, carbon, and optionally additionally doped with hydrogen.
- the carrier metal oxide on the first metal lattice sites is preferably doped with at least one element from the group comprising iridium and ruthenium.
- the catalyst material has, in particular, a second crystal lattice structure comprising second oxygen lattice sites and second metal lattice sites, the catalyst material on the second oxygen lattice sites being doped with at least one element from the group comprising: fluorine, nitrogen, carbon, boron and optionally additionally being doped with Hydrogen.
- the catalyst material on the second metal grid positions is preferably doped with at least one element from the group comprising iridium, ruthenium, iron, tungsten, cobalt, nickel, molybdenum, vanadium, platinum, palladium. In total, this also serves in particular to adjust the electrical conductivity of the metal phosphate.
- the carrier metal oxide and the catalyst material are adjusted with different surface energies, so that their wetting behavior with respect to water is different. It has proven to be advantageous if the catalyst material is more hydrophilic than the carrier metal oxide, in particular that the catalyst material is hydrophilic and the carrier metal oxide is hydrophobic. Alternatively, however, it is also possible for the catalyst material to be hydrophobic and for the support metal oxide to be hydrophilic.
- the properties are stabilized and adjusted by a combined process of fluorinating and / or nitriding and / or carbonizing and / or boronizing.
- a combined process of fluorinating and / or nitriding and / or carbonizing and / or boronizing are set, while the other doping elements adjust the conductivity and the surface energy states.
- Non-conductors become electrical conductors, or the particles have a high ionic conductivity or they adsorb specific atoms / molecules on the surface.
- the following principles apply to recruitment:
- electrical insulators can be converted to highly conductive materials; S1O2, for example, is a strong adsorbent for negative charges, so that the F conductivity in fluorides can be significantly increased in this way;
- the effects can be controlled efficiently by doping surface-active phases, here in particular to adjust the metal phosphate in contact with the nanoscale carrier metal oxide. Platinum is preferably applied to a surface of the electrode in a maximum amount of 0.1 mg / cm 2 (based on a projected electrode area).
- the polymer electrolyte membrane and an ionomer contained in the electrode are formed in particular from identical materials.
- Example 1 Conductive carrier metal oxide with zirconium phosphate (with platinum doping)
- Tin dioxide with 0.9 at% tantalum oxide Ta20s was produced as the carrier metal oxide.
- concentration setting of the Ta20 in the tin dioxide was in the alpha solubility of the tantalum oxide in the tin oxide.
- the electrical conductivity of the carrier metal oxide was determined on a powder compact as 6.5 x 10 2 Sem -2 .
- the particle size of the carrier metal oxide was between 75 and 100 nm.
- the metal phosphate in the form of zirconium phosphate was first made from zirconium tartrate by reaction with concentrated phosphoric acid. The precipitated salt was washed thoroughly, dried and calcined at 400 ° C under nitrogen. The powder obtained was ground to a particle size of 10 to 20 nm using a high-energy mill.
- the metal phosphate and the carrier metal oxide were intimately mixed in a ratio of 1:10 and then mixed for better contacting in a ball mill at a low number of revolutions.
- the powder obtained was sputtered with platinum on a rotating substrate plate by means of a sputtering process.
- the platinum particles had a particle size in the range from 2 to 4 nm, the amount of platinum being about 0.1 mgpt / cm 2 with a layer thickness applied at 10 pm.
- the catalyst system was initially qualified using RDE. For this purpose, a 1 pm thick, Nafion-bound layer was applied to glassy carbon. The qualification was carried out as standard with revolutions of the RDE of 1600 rpm in 0.1 M HCIO4 at 60 ° C. The voltage cycle or a “sweep rate” was between 1300 mV and 300 mV compared to NHE is 20 mV / s.
- the diffusion-determined limit current of the sample was 5.8 mA / cm 2.
- the limit current was reached at 710 mV compared to NHE.
- the catalyst system was tested on a 50 cm 2 Nafion film (Gore) with a single cell.
- the catalyst system was mixed with the ionomer (20% by weight Nafion solution (1000EW, Dupont)) and isopropanol and applied to a gas diffusion layer comprising an MPL (MicroPorousLayer) layer (SGL) in the CCS process.
- MPL MicroPorousLayer
- the layer thickness was 10 pm ⁇ 0.5 pm.
- the catalyst system tended to agglomerate during application of the dispersion to the Nafion film.
- Example 2 Conductive fluorine-treated carrier metal oxide with zirconium phosphate
- the carrier metal oxide was produced as described for Example 1. The only difference was that the carrier metal oxide was treated with fluorine after production at 700 ° C. Already after removal from the furnace, the carrier metal oxide showed a much better flow than before. All of the following steps corresponded to those described in Example 1 above. The fluorination resulted in a slightly reduced electrical conductivity of the carrier metal oxide at a value of 3 ⁇ 10 2 S / cm 2 .
- the onset voltage for the acid reduction was 980 mV compared to NHE, and 1.2 A & 0.69 V are achieved in the single cell. After a load time of more than 500 h and repeated CV checks, no significant change in the characteristic data was found.
- Example 3 Conductive fluorine-treated carrier metal oxide with tantalum phosphate
- the carrier metal oxide was produced according to Example 2.
- the metal phosphate in the form of tantalum phosphate was again made from a tartrate complex with ammonium dihydrogen phosphate.
- the tantalum phosphate was mixed intensively with the carrier metal oxide in a ball mill. For better comparability, a mixing ratio of 1:10 as in Example 1 was also chosen.
- the platinum was applied to the powder evenly using a sputtering process. Surprisingly good results were achieved with this catalyst system, an onset voltage for oxygen reduction of 1100 mV compared to NHE and 1.2 A & 0.75 V being achieved in the single cell. The hydrolysis stability was again verified over 500 h without a noticeable drop in the specific data.
- the manner in which the carrier metal oxide is coated with metal phosphate and the mixing of carrier metal oxide and metal phosphate have a strong influence on the characteristics of the catalyst system.
- the catalyst system also has a much higher stability. Significant effects could be achieved if the acidic catalyst material was adjusted to grain sizes below 2 nm.
- the “coherent” adsorption of the metal phosphate on the surface of the carrier metal oxide enables a changed electronic structure with the influence of favorable field strength effects between the catalyst material and the carrier metal oxide.
- FIG. 3 shows a section III-III through the arrangement according to FIG. 1;
- FIG. 1 shows an electrode 1 on a bipolar plate 2, which has a carrier plate 2a.
- the electrode 1 contains the catalyst system 9 (see FIG. 3) and forms a cathode.
- the electrode 1 has a layer thickness in the range from 1 to 2 pm and in addition to the catalyst system 9 further comprises an ionomer and a binder, here in the form of agar-agar.
- the bipolar plate 2 has an inflow area 3a with openings 4 and an outlet area 3b with further openings 4 ' , which serve to supply a fuel cell with process gases and to remove reaction products from the fuel cell.
- the bipolar plate 2 furthermore has a gas distributor structure 5 on each side, which is provided for contact with a polymer electrolyte membrane 7 (see FIG. 2).
- FIG. 2 schematically shows a fuel cell system 100 comprising a plurality of fuel cells 10.
- Each fuel cell 10 comprises a polymer electrolyte membrane 7, which is adjacent on both sides by bipolar plates 2, 2 ' .
- the same reference numerals as in FIG 1 denote the same elements.
- FIG. 3 shows a section III-III through the electrochemical single cell 2 according to FIG. 1.
- the same reference numerals as in FIG. 1 denote the same elements.
- the carrier plate 2a which is formed here from stainless steel, can be seen, which can be constructed in one part or in several parts.
- a gas diffusion layer 6 is arranged between the carrier plate 2a and the electrode 1, which contains the catalyst system 9. Furthermore, it can be seen that a further anode-side coating 8 of the carrier plate 2a is present. This is preferably a coating 8, which is designed according to DE 10 2016 202 372 A1.
- the Gasdif fusion layers 6, 6 ' are electrically conductive.
- FIG. 4 shows a section through two bipolar plates 2, 2 ' and an interposed polymer electrolyte membrane 7 according to FIG. 2, which together form a fuel cell 10.
- the same reference numerals as in Figures 1 to 3 denote the same elements. It can be seen that the electrode 1 of the bipolar plate 2 as the cathode and on the other hand the coating 8 of the bipolar plate 2 ' as the anode are arranged adjacent to the polymer electrolyte membranes 7. Furthermore, the gas diffusion layers 6, 6 'can be seen .
- a catalyst system 9 is presented using the example of the quasibinary oxide phase diagram Ta205-Sn02 for the carrier metal oxide.
- the mutual solubilities towards lower temperatures have to be extrapolated and estimated. From the phase diagram it can be seen that tin oxide in tantalum oxide has an initial solubility of about 7 mol% at the temperature mentioned, while the initial solubility of tantalum oxide in tin oxide is 1.1 mol%. Accordingly, it can be assumed that the solubilities are lower at room temperature or at the operating temperature of a fuel cell.
- the course of activity of the two oxides at 1500 ° C. in the respective mixed phases is shown in FIG. 6 (J. Am. Ceram. Soc., 95 [12], 4004-4007, (2012)).
- the stable thorelaurite phase SnTa207 is not included in this phase diagram according to FIG. 6.
- the tin is tetravalent in this compound.
- With the solid solution of tin oxide with tantalum oxide the electrical conductivity of the tin oxide becomes drastic elevated.
- tantalum oxide up to the maximum a solubility of 1.1 mol% to tin oxide, electrical conductivities of 7x10 2 S / cm 2 are achieved.
- the composition of the heterogeneous structure can be calculated at given concentrations according to the lever law. If, for example, a total concentration of 10 mol% Ta20s in Sn02 is selected, the result is a composition of the heterogeneous structure of 88% Sno, 99Tao, oi02 and 2% SnTa207 as oxide composite.
- the conductivity of the tin oxide in which the tantalum oxide is dissolved to the maximum limit solubility (approx. 1.1 mol%), depends heavily on the sintering temperature. It is important to ensure that the oxygen partial pressure above the powder is always high enough so that the fully oxidized compounds are formed. Otherwise post-oxidation during cell operation and loss of electrochemical activity can be expected.
- the carrier metal oxide was subjected to a nitrogen treatment and / or a carbon treatment (in particular with C2H2) and / or fluorinated with the aid of CF4. Exceptionally good results have already been achieved with the carbon or nitrogen-treated carrier metal oxides.
- a tantalum phosphate was mixed with the carrier metal oxide as the metal phosphate. It was also investigated how a further deposition of nanodisperse platinum particles affects the electrocatalytic effectiveness of the catalyst system.
- the platinum was deposited using sputtering technology with an area coverage of ⁇ 0.1 mg / cm 2 on the surface of the catalyst system No. 4 according to Table 2. In this catalyst system with platinum, surprisingly high activities for oxygen reduction were found. Overall, it can be stated that surprisingly high activities for oxygen reduction are found in the embodiments of the catalyst system according to the invention both without platinum and with platinum. Similar results were obtained with the same-type niobium-containing tin oxide composites. Niobium oxide has a somewhat higher solubility in tin oxide than tantalum oxide.
- the limit solubility for niobium oxide is 2.5 at .-%.
- niobium oxide similar stable stoichiometric phases SnNb207 (“Froodite”) are formed as the thoreaulite phase.
- the measured activities are lower than with the tantalum-based catalyst systems, which can be explained, among other things, by different pzzp values. However, it should be noted at this point that the activities depend very much on the manufacturing conditions.
Abstract
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DE102019133872.7A DE102019133872A1 (en) | 2018-12-19 | 2019-12-11 | Fuel cell or electrolyzer |
PCT/DE2019/101077 WO2020125861A1 (en) | 2018-12-19 | 2019-12-12 | Fuel cell or electrolyser |
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JP4438283B2 (en) * | 2002-12-03 | 2010-03-24 | 旭硝子株式会社 | Membrane electrode assembly |
MY143356A (en) * | 2004-06-25 | 2011-04-29 | Very Small Particle Company Pty Ltd | Method for producing fine-grained particles |
JP2006210135A (en) * | 2005-01-28 | 2006-08-10 | Sony Corp | Catalyst electrode material, catalyst electrode, manufacturing method thereof, support material for electrode catalyst and electrochemical device |
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US8062552B2 (en) * | 2005-05-19 | 2011-11-22 | Brookhaven Science Associates, Llc | Electrocatalyst for oxygen reduction with reduced platinum oxidation and dissolution rates |
KR100879299B1 (en) * | 2007-06-20 | 2009-01-19 | 삼성에스디아이 주식회사 | Catalyst for cathod of mixed reactant fuel cell, and membrane-electrode assembly for mixed reactant fuel cell and mixed reactant fuel cell system including same |
JP5274149B2 (en) * | 2008-08-20 | 2013-08-28 | キヤノン株式会社 | Fuel cell |
US20110136047A1 (en) * | 2008-09-19 | 2011-06-09 | Belabbes Merzougui | Fuel cell catalyst support with boron carbide-coated metal oxides/phosphates and method of manufacturing same |
JP2010108914A (en) * | 2008-10-02 | 2010-05-13 | Nissan Motor Co Ltd | Fuel cell, and operation method thereof |
US9252431B2 (en) * | 2009-02-10 | 2016-02-02 | Audi Ag | Fuel cell catalyst with metal oxide/phosphate support structure and method of manufacturing same |
US9065141B2 (en) * | 2009-02-10 | 2015-06-23 | Audi Ag | Boron-doped diamond coated catalyst support |
JP2013524442A (en) * | 2010-04-01 | 2013-06-17 | トレナージ コーポレーション | High temperature membrane / electrode assembly having high power density and corresponding manufacturing method |
US8273679B2 (en) * | 2010-09-24 | 2012-09-25 | National Central University | Porous catalyst for a fuel cell and method for producing the catalyst thereof |
JP2012104244A (en) * | 2010-11-05 | 2012-05-31 | Kuraray Co Ltd | Composition for forming catalyst layer, gas diffusion electrode, membrane-electrode assembly and fuel cell |
US10041179B2 (en) * | 2012-08-08 | 2018-08-07 | University of Pittsburgh—of the Commonwealth System of Higher Education | Non-noble metal based electro-catalyst compositions for proton exchange membrane based water electrolysis and methods of making |
JP5994729B2 (en) * | 2013-05-24 | 2016-09-21 | トヨタ自動車株式会社 | A fuel cell catalyst electrode layer, a membrane electrode assembly, a fuel cell, and a method for producing a fuel cell catalyst electrode layer. |
GB201322494D0 (en) * | 2013-12-19 | 2014-02-05 | Johnson Matthey Fuel Cells Ltd | Catalyst layer |
WO2015124250A1 (en) * | 2014-02-20 | 2015-08-27 | Merck Patent Gmbh | Stable catalyst ink formulations, methods of using such inks in fiber formation, and articles comprising such fibers |
DE102014205033A1 (en) * | 2014-03-18 | 2015-09-24 | Volkswagen Ag | Catalyst layer for a fuel cell and method for producing such |
JP6331580B2 (en) * | 2014-03-28 | 2018-05-30 | 日揮触媒化成株式会社 | Electrode catalyst, catalyst layer precursor, catalyst layer, and fuel cell |
GB201415846D0 (en) * | 2014-09-08 | 2014-10-22 | Johnson Matthey Fuel Cells Ltd | Catalyst |
DE102015101249B4 (en) | 2014-12-01 | 2021-02-11 | Deutsches Zentrum für Luft- und Raumfahrt e.V. | A method for producing an electrocatalyst for an electrode of an electrochemical cell, an electrochemical reactor and an electrocatalyst for an electrochemical cell |
US20160204442A1 (en) * | 2015-01-08 | 2016-07-14 | Nissan North America, Inc. | Mixed-metal oxide catalyst layer with sacrificial material |
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JP2017162572A (en) * | 2016-03-07 | 2017-09-14 | 日揮触媒化成株式会社 | Electrode catalyst, carrier used therefor and method for manufacturing the same, and fuel battery using the electrode catalyst |
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