WO2023089602A1 - Solid oxide fuel cell arrangement generating ammonia as byproduct and utilizing ammonia as secondary fuel - Google Patents
Solid oxide fuel cell arrangement generating ammonia as byproduct and utilizing ammonia as secondary fuel Download PDFInfo
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- WO2023089602A1 WO2023089602A1 PCT/IL2021/051365 IL2021051365W WO2023089602A1 WO 2023089602 A1 WO2023089602 A1 WO 2023089602A1 IL 2021051365 W IL2021051365 W IL 2021051365W WO 2023089602 A1 WO2023089602 A1 WO 2023089602A1
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- ammonia
- fuel cell
- cell arrangement
- anode
- fed
- Prior art date
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- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 title claims abstract description 125
- 239000000446 fuel Substances 0.000 title claims abstract description 73
- 229910021529 ammonia Inorganic materials 0.000 title claims abstract description 62
- 239000007787 solid Substances 0.000 title claims abstract description 17
- 239000006227 byproduct Substances 0.000 title claims abstract description 14
- 239000007789 gas Substances 0.000 claims abstract description 39
- 239000001257 hydrogen Substances 0.000 claims abstract description 22
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 22
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 21
- IJGRMHOSHXDMSA-UHFFFAOYSA-N nitrogen Substances N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 21
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims abstract description 16
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims abstract description 16
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims abstract description 16
- 239000004215 Carbon black (E152) Substances 0.000 claims abstract description 13
- 229930195733 hydrocarbon Natural products 0.000 claims abstract description 13
- 150000002430 hydrocarbons Chemical class 0.000 claims abstract description 13
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 13
- 229910052706 scandium Inorganic materials 0.000 claims abstract description 12
- SIXSYDAISGFNSX-UHFFFAOYSA-N scandium atom Chemical compound [Sc] SIXSYDAISGFNSX-UHFFFAOYSA-N 0.000 claims abstract description 12
- 229910052723 transition metal Inorganic materials 0.000 claims abstract description 11
- 150000003624 transition metals Chemical class 0.000 claims abstract description 11
- 229910052684 Cerium Inorganic materials 0.000 claims abstract description 9
- 239000003792 electrolyte Substances 0.000 claims abstract description 9
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims abstract description 8
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims abstract description 8
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims abstract description 8
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 claims abstract description 8
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims abstract description 8
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims abstract description 8
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims abstract description 8
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims abstract description 8
- 229910052804 chromium Inorganic materials 0.000 claims abstract description 8
- 239000011651 chromium Substances 0.000 claims abstract description 8
- 229910017052 cobalt Inorganic materials 0.000 claims abstract description 8
- 239000010941 cobalt Substances 0.000 claims abstract description 8
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims abstract description 8
- 229910052802 copper Inorganic materials 0.000 claims abstract description 8
- 239000010949 copper Substances 0.000 claims abstract description 8
- 229910052742 iron Inorganic materials 0.000 claims abstract description 8
- 229910052746 lanthanum Inorganic materials 0.000 claims abstract description 8
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 claims abstract description 8
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims abstract description 8
- 229910052750 molybdenum Inorganic materials 0.000 claims abstract description 8
- 239000011733 molybdenum Substances 0.000 claims abstract description 8
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 8
- 229910052758 niobium Inorganic materials 0.000 claims abstract description 8
- 239000010955 niobium Substances 0.000 claims abstract description 8
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims abstract description 8
- 229910052763 palladium Inorganic materials 0.000 claims abstract description 8
- 229910052703 rhodium Inorganic materials 0.000 claims abstract description 8
- 239000010948 rhodium Substances 0.000 claims abstract description 8
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims abstract description 8
- 229910052707 ruthenium Inorganic materials 0.000 claims abstract description 8
- 229910052719 titanium Inorganic materials 0.000 claims abstract description 8
- 239000010936 titanium Substances 0.000 claims abstract description 8
- 229910052720 vanadium Inorganic materials 0.000 claims abstract description 8
- 229910052727 yttrium Inorganic materials 0.000 claims abstract description 8
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 claims abstract description 8
- 229910052725 zinc Inorganic materials 0.000 claims abstract description 8
- 239000011701 zinc Substances 0.000 claims abstract description 8
- 229910052726 zirconium Inorganic materials 0.000 claims abstract description 8
- 239000011195 cermet Substances 0.000 claims abstract description 7
- 230000005611 electricity Effects 0.000 claims abstract description 7
- 239000000203 mixture Substances 0.000 claims abstract description 7
- AHKZTVQIVOEVFO-UHFFFAOYSA-N oxide(2-) Chemical compound [O-2] AHKZTVQIVOEVFO-UHFFFAOYSA-N 0.000 claims abstract description 4
- ZMIGMASIKSOYAM-UHFFFAOYSA-N cerium Chemical compound [Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce] ZMIGMASIKSOYAM-UHFFFAOYSA-N 0.000 claims description 8
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 claims description 7
- 239000006096 absorbing agent Substances 0.000 claims description 5
- 230000003197 catalytic effect Effects 0.000 claims description 5
- 239000012528 membrane Substances 0.000 claims description 4
- 238000000034 method Methods 0.000 claims description 4
- 150000001875 compounds Chemical class 0.000 claims description 3
- 239000000470 constituent Substances 0.000 claims description 3
- 238000005086 pumping Methods 0.000 claims description 2
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 abstract 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 abstract 1
- 238000010586 diagram Methods 0.000 description 5
- 239000003054 catalyst Substances 0.000 description 3
- 238000012986 modification Methods 0.000 description 3
- 230000004048 modification Effects 0.000 description 3
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonium chloride Substances [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 description 2
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 2
- 229910052688 Gadolinium Inorganic materials 0.000 description 2
- 235000011114 ammonium hydroxide Nutrition 0.000 description 2
- 229910000420 cerium oxide Inorganic materials 0.000 description 2
- 238000012512 characterization method Methods 0.000 description 2
- UIWYJDYFSGRHKR-UHFFFAOYSA-N gadolinium atom Chemical compound [Gd] UIWYJDYFSGRHKR-UHFFFAOYSA-N 0.000 description 2
- 150000002431 hydrogen Chemical class 0.000 description 2
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 2
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 229910001928 zirconium oxide Inorganic materials 0.000 description 2
- QESCUTSFWAZEMC-UHFFFAOYSA-N [Ni]=O.[O-2].[Zr+4].[O-2] Chemical compound [Ni]=O.[O-2].[Zr+4].[O-2] QESCUTSFWAZEMC-UHFFFAOYSA-N 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- LBSANEJBGMCTBH-UHFFFAOYSA-N manganate Chemical compound [O-][Mn]([O-])(=O)=O LBSANEJBGMCTBH-UHFFFAOYSA-N 0.000 description 1
- IOKPLNQRQWZPGF-UHFFFAOYSA-N nickel(2+);oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[O-2].[Ni+2].[Zr+4] IOKPLNQRQWZPGF-UHFFFAOYSA-N 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 238000002407 reforming Methods 0.000 description 1
- 239000012465 retentate Substances 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- IGPAMRAHTMKVDN-UHFFFAOYSA-N strontium dioxido(dioxo)manganese lanthanum(3+) Chemical compound [Sr+2].[La+3].[O-][Mn]([O-])(=O)=O IGPAMRAHTMKVDN-UHFFFAOYSA-N 0.000 description 1
- 238000013022 venting Methods 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
- C01B3/047—Decomposition of ammonia
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01C—AMMONIA; CYANOGEN; COMPOUNDS THEREOF
- C01C1/00—Ammonia; Compounds thereof
- C01C1/02—Preparation, purification or separation of ammonia
- C01C1/04—Preparation of ammonia by synthesis in the gas phase
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01C—AMMONIA; CYANOGEN; COMPOUNDS THEREOF
- C01C1/00—Ammonia; Compounds thereof
- C01C1/02—Preparation, purification or separation of ammonia
- C01C1/04—Preparation of ammonia by synthesis in the gas phase
- C01C1/0405—Preparation of ammonia by synthesis in the gas phase from N2 and H2 in presence of a catalyst
- C01C1/0458—Separation of NH3
-
- 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
- H01M4/9041—Metals or alloys
- H01M4/905—Metals or alloys specially used in fuel cell operating at high temperature, e.g. SOFC
- H01M4/9066—Metals or alloys specially used in fuel cell operating at high temperature, e.g. SOFC of metal-ceramic composites or mixtures, e.g. cermets
-
- 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
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
- H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
-
- 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
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
- H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
- H01M8/04111—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants using a compressor turbine assembly
-
- 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
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
- H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
- H01M8/04119—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with simultaneous supply or evacuation of electrolyte; Humidifying or dehumidifying
-
- 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
- H01M8/1231—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte with both reactants being gaseous or vaporised
-
- 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 fuel cells and, more particularly, high-temperature solid oxide fuel cells to generate electricity and ammonia as a byproduct available for further use.
- Fuel cells are electrochemical devices that convert the chemical energy of fuel and an oxidizing agent into electricity. Hydrogen or substances that include hydrogen are used as fuel in fuel cells.
- the fuel cells where ammonia is directly fed to an anode of the fuel cell are known in the art (see, for example, US7157166).
- An alternative technical solution concerns the fuel cells fueled by hydrogen generated in the decomposition of ammonia fuel into hydrogen and nitrogen (US3532547).
- WO/2020/141500 discloses a high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel and generating electricity and ammonia as a byproduct.
- the arrangement comprises (a) a cathode area fed with air; (b) an anode area fed with the fuel; and (c) an oxide ion-conducting electrolyte disposed between the cathode and anode areas.
- the cathode has an ammonia-rich tail-gas stream.
- the fuel cell further comprises a gas separator configured for separating ammonia generated on the cathode from tail-gas stream and means for utilizing separated ammonia selected from the group consisting of an ammonia reformer configured for generating hydrogen to be admixed to the fuel fed to the anode, a collecting tank for storing the ammonia and an auxiliary solid oxide fuel cell fueled by the separated ammonia and any combination thereof.
- a gas separator configured for separating ammonia generated on the cathode from tail-gas stream and means for utilizing separated ammonia selected from the group consisting of an ammonia reformer configured for generating hydrogen to be admixed to the fuel fed to the anode, a collecting tank for storing the ammonia and an auxiliary solid oxide fuel cell fueled by the separated ammonia and any combination thereof.
- An aspect of the present invention relates to a high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel and generating electricity and ammonia as a byproduct.
- the aforesaid fuel cell comprises: (a) a cathode area fed with dry air; (b) an anode area fed with said fuel; and (c) an oxide ion-conducting electrolyte area disposed between said cathode and anode areas.
- It is a core purpose of the invention is to provide the anode area comprising transition metals selected from the group consisting of Lanthanum, Cerium, Scandium, Titanium, Vanadium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Ruthenium, Rhodium, Palladium, Argentum and any combination thereof; n.
- the anode area when fed with a hydrogen (H2) and nitrogen (N2) mixture generates exhausted gases comprising gaseous ammonia.
- a further object of the invention is to disclose the anode area comprising a cermet Ni-ScSZ layer and a catalytic layer.
- a further object of the invention is to disclose the catalytic layer comprising a compound of transition metals and nitrogen ⁇ TM ⁇ oTM ⁇ TM ⁇ N y where i and xi are positive integers; said transition metals are selected from the group consisting of Lanthanum, Cerium, Scandium, Titanium, Vanadium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Ruthenium, Rhodium, Palladium, Argentum and any combination thereof.
- a further object of the invention is to disclose the fuel cell arrangement comprising a gas separator.
- a further object of the invention is to disclose the gas separator comprising a compressor configured for pressurizing said exhausted gases.
- a further object of the invention is to disclose the compressor said compressor configured for pumping said exhausted gases via a membrane arrangement such that ammonia is separated from said exhausted gases.
- a further object of the invention is to disclose the compressor configured for liquefying said gaseous ammonia while other constituents of the exhausted gases are vented to the atmosphere.
- a further object of the invention is to disclose the gas separator comprising an ammonia absorber and an ammonia evaporator heated by heat generated by said fuel cell.
- a further object of the invention is to disclose a method of generating ammonia as a byproduct by a high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel; said method comprising steps of: (a) providing a high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel; said fuel cell comprising: (i) a cathode area fed with a air; (ii) an anode area said comprising transition metals selected from the group consisting of Lanthanum, Cerium, Scandium, Titanium, Vanadium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Ruthenium, Rhodium, Palladium, Argentum and any combination thereof and (iii) an oxide ion-conducting electrolyte disposed between said cathode and anode areas; said anode comprises a cermet Ni- ScSZ layer and a
- Fig. 1 is a schematic diagram of a high-temperature solid oxide fuel cell arrangement
- Fig. 2 is a schematic diagram of a high-temperature solid oxide fuel cell arrangement provided with an ammonia reformer
- Fig. 3 is a detailed schematic diagram of a dephlegmator-based separator
- Fig. 4 is a detailed schematic diagram of a membrane -based separator
- Fig. 5 is a detailed schematic diagram of an expansion-based separator. DETAILED DESCRIPTION OF THE INVENTION
- Figs 1 and 2 presenting alternative embodiments of high-temperature solid oxide fuel cell arrangement 100a to 100b fueled by a hydrogen or hydrocarbon fuel to anode fuel cell and dry air to the cathode and generating ammonia as a byproduct on the anode of the fuel cell.
- Arrangements 100a and 100b include gas separator 130, which separates gaseous ammonia exhausted gases fed to separator 130 via passage 131.
- Numeral 140 marks electric energy provided by fuel cell 110 to a load (not shown).
- Anode area 113 is fluidly connected to separator 130 by passage 131.
- Anode area 113 is made of a cermet comprising transition metals such as Lanthanum, Cerium, Scandium, Titanium, Vanadium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Ruthenium, Rhodium, Palladium and Argentum.
- anode area 113 is provided with a catalyst layer (not shown) made of made of a compound of transition metals and nitrogen ⁇ TM ⁇ oTM ⁇ TM ⁇ N y where i and xi are positive integers Exhausting gases from cathode area 117 are vented to atmosphere.
- Feeding dry air to cathode area 117, generating gaseous ammonia therewithin and feeding the exhausting gases containing ammonia to separator 130 is also in the scope of the present invention.
- Electric energy generated by fuel cell 110 is designated by numeral 127.
- the heat generated in fuel cell 110 is transferred to separator 130 via passage 131.
- ammonia separated from exhausted gases is fed to ammonia tank 140 via passage 135.
- Arrangement 100b (Fig. 2), separated ammonia is fed to reformer 150 via passage 151.
- After reforming, obtained hydrogen and nitrogen are admixed via passages 153 and 155 to hydrogen or any hydrocarbon fuel fed to anode area 113 via passage 121.
- Embodiment 150a in Fig. 3 includes ammonia absorber 270, ammonia evaporator 280 and dephlegmator 290.
- the exhausted gases are fed into ammonia absorber 270 via passage 131 based on absorbing ammonia from the exhausting gases in water.
- An ammonia solution obtained in absorber 270 then is fed into ammonia evaporator 280 via passage 275.
- the aqueous ammonia solution is vaporized by the heat generated by fuel cell 110 (not shown) via heat transfer means 129.
- the vapor generated within ammonia evaporator 280 via passage 285 is provided to dephlegmator 290 where ammonia and water vapor fractions are separated. Separated ammonia outputs via passage 295.
- the exhausted gases via passage 131 are collected in tank 210 configured for storing exhausted tail gases.
- the exhausted gases stored in tank 210 are then pumped by compressor 220 via passages 215 and 225 and fed to membrane arrangement 260 configured for separating ammonia from the aforesaid exhausted gases. Separated ammonia (permeant gas) outputs from passage 265.
- Passage 265 is designed for venting retentate gases.
- FIG. 5 embodiment 200c is presented.
- the gases exhausted from the anode area (not shown) are fed to tank 210 via passage 131.
- Tank 230 is configured for accumulating the aforesaid exhausted gases.
- the exhausted gases via passage 215 reach compressor 220 is used for pressurizing the exhausted gases.
- the pressurization of the exhausted gasses results in liquefying ammonia which is accumulated via passage 225 in tank 230 while other constituents of the pressurized gases are vented to the atmosphere via passage 235.
- Ammonia is cooled when it passes via expansion valve 240. Thereat, low-temperature gaseous ammonia can be used for cooling a working body circulating in loop 255 in heat-exchange arrangement 253.
- gaseous ammonia is provided via pipe 155 to a consumer.
- Cathode Eanthanum-Strontium Manganate/Cerium oxide doped with Gadolinium.
- Electrolyte Zirconium oxide stabilized by Scandium
- Anode Nickel oxide-Zirconium oxide stabilized by Scandium.
- the fuel cell was fed with hydrogen and nitrogen (1:1 ratio) with flow rate of 0.4 1/min at the anode and air at the cathode with flow rate of 1 1/min. Operation temperature was about 800°C.
- Cathode Lanthanum-Strontium Manganate/Cerium oxide doped with Gadolinium.
- Electrolyte Zirconium oxide stabilized by Scandium and Cerium
- Anode Nickel-Zirconium oxide stabilized by Scandium provided with a layer of catalyst MmN.
- the catalyst layer is coated onto the anode by means of serigraphic deposition
- the fuel cell was fed with hydrogen and nitrogen (1: 1 ratio) with flow rate 0.4 l/min at the anode and air at the cathode with flow rate of 1 1/min. Operation temperature was about 800°C. The results of characterization are in Table 1.
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- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Inorganic Chemistry (AREA)
- Analytical Chemistry (AREA)
- Materials Engineering (AREA)
- Health & Medical Sciences (AREA)
- General Health & Medical Sciences (AREA)
- Combustion & Propulsion (AREA)
- Composite Materials (AREA)
- Ceramic Engineering (AREA)
- Catalysts (AREA)
- Fuel Cell (AREA)
Abstract
A high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel and generating electricity and ammonia as a byproduct comprises: a cathode area fed with air, an anode area fed with said fuel and an oxide ion -conducting electrolyte area disposed between said cathode and anode areas. The anode area is made of cermet comprising transition metals selected from the group consisting of Lanthanum, Cerium, Scandium, Titanium, Vanadium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Ruthenium, Rhodium, Palladium, Argentum and any combination thereof; said anode area when fed with a hydrogen-nitrogen mixture generates exhausted gases comprising gaseous ammonia.
Description
SOLID OXIDE FUEL CELL ARRANGEMENT GENERATING AMMONIA AS BYPRODUCT AND UTILIZING AMMONIA AS SECONDARY FUEL
FIELD OF THE INVENTION
The present invention relates to fuel cells and, more particularly, high-temperature solid oxide fuel cells to generate electricity and ammonia as a byproduct available for further use.
BACKGROUND OF THE INVENTION
Fuel cells are electrochemical devices that convert the chemical energy of fuel and an oxidizing agent into electricity. Hydrogen or substances that include hydrogen are used as fuel in fuel cells. The fuel cells where ammonia is directly fed to an anode of the fuel cell are known in the art (see, for example, US7157166). An alternative technical solution concerns the fuel cells fueled by hydrogen generated in the decomposition of ammonia fuel into hydrogen and nitrogen (US3532547).
WO/2020/141500 discloses a high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel and generating electricity and ammonia as a byproduct. The arrangement comprises (a) a cathode area fed with air; (b) an anode area fed with the fuel; and (c) an oxide ion-conducting electrolyte disposed between the cathode and anode areas. The cathode has an ammonia-rich tail-gas stream. The fuel cell further comprises a gas separator configured for separating ammonia generated on the cathode from tail-gas stream and means for utilizing separated ammonia selected from the group consisting of an ammonia reformer configured for generating hydrogen to be admixed to the fuel fed to the anode, a collecting tank for storing the ammonia and an auxiliary solid oxide fuel cell fueled by the separated ammonia and any combination thereof.
The high-temperature solid oxide fuel cells fed with hydrogen or hydrocarbon fuels enabling utilization of ammonia generated as a byproduct at the cathode area are known in the art. Thus, there is a long-felt need for providing fuel cells generating ammonia in a more effective manner at the anode with a higher ammonia output.
SUMMARY OF THE INVENTION
An aspect of the present invention relates to a high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel and generating electricity and ammonia as a byproduct. The aforesaid fuel cell comprises: (a) a cathode area fed with dry air; (b) an anode area fed with said fuel; and (c) an oxide ion-conducting electrolyte area disposed between said cathode and anode areas.
It is a core purpose of the invention is to provide the anode area comprising transition metals selected from the group consisting of Lanthanum, Cerium, Scandium, Titanium, Vanadium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Ruthenium, Rhodium, Palladium, Argentum and any combination thereof; n. The anode area when fed with a hydrogen (H2) and nitrogen (N2) mixture generates exhausted gases comprising gaseous ammonia.
A further object of the invention is to disclose the anode area comprising a cermet Ni-ScSZ layer and a catalytic layer.
A further object of the invention is to disclose the catalytic layer comprising a compound of transition metals and nitrogen {TM^oTM^ TM^ Ny where i and xi are positive integers; said transition metals are selected from the group consisting of Lanthanum, Cerium, Scandium, Titanium, Vanadium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Ruthenium, Rhodium, Palladium, Argentum and any combination thereof.
A further object of the invention is to disclose the fuel cell arrangement comprising a gas separator.
A further object of the invention is to disclose the gas separator comprising a compressor configured for pressurizing said exhausted gases.
A further object of the invention is to disclose the compressor said compressor configured for pumping said exhausted gases via a membrane arrangement such that ammonia is separated from said exhausted gases.
A further object of the invention is to disclose the compressor configured for liquefying said gaseous ammonia while other constituents of the exhausted gases are vented to the atmosphere.
A further object of the invention is to disclose the gas separator comprising an ammonia absorber and an ammonia evaporator heated by heat generated by said fuel cell.
A further object of the invention is to disclose a method of generating ammonia as a byproduct by a high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel; said method comprising steps of: (a) providing a high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel; said fuel cell comprising: (i) a cathode area fed with a air; (ii) an anode area said comprising transition metals selected from the group consisting of Lanthanum, Cerium, Scandium, Titanium, Vanadium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Ruthenium, Rhodium, Palladium, Argentum and any combination thereof and (iii) an oxide ion-conducting electrolyte disposed between said cathode and anode areas; said anode comprises a cermet Ni- ScSZ layer and a M N catalytic layer; said anode area being fed with an hydrogen-nitrogen mixture generates exhausted gases comprising gaseous ammonia; (b) feeding said fuel-nitrogen mixture to said anode area; (c) feeding air to said cathode area; (d) operating said fuel cell; (e) generating said ammonia as a byproduct in said anode area; and (f) separating said ammonia from said exhausted stream.
BRIEF DESCRIPTION OF THE DRAWINGS
In order to understand the invention and to see how it may be implemented in practice, a plurality of embodiments is adapted to now be described, by way of non-limiting example only, with reference to the accompanying drawings, in which:
Fig. 1 is a schematic diagram of a high-temperature solid oxide fuel cell arrangement;
Fig. 2 is a schematic diagram of a high-temperature solid oxide fuel cell arrangement provided with an ammonia reformer;
Fig. 3 is a detailed schematic diagram of a dephlegmator-based separator;
Fig. 4 is a detailed schematic diagram of a membrane -based separator; and
Fig. 5 is a detailed schematic diagram of an expansion-based separator.
DETAILED DESCRIPTION OF THE INVENTION
The following description is provided, so as to enable any person skilled in the art to make use of said invention and sets forth the best modes contemplated by the inventor of carrying out this invention. Various modifications, however, are adapted to remain apparent to those skilled in the art since the generic principles of the present invention have been defined specifically to provide high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel and generating electricity and ammonia as a byproduct.
Reference is now made to Figs 1 and 2 presenting alternative embodiments of high-temperature solid oxide fuel cell arrangement 100a to 100b fueled by a hydrogen or hydrocarbon fuel to anode fuel cell and dry air to the cathode and generating ammonia as a byproduct on the anode of the fuel cell.
Referring to Figs 1 and 2, hydrogen or any hydrocarbon fuel is fed to anode area 113 of fuel cell 110 via passage 121. Concurrently, air is fed to cathode area 117 via passage 123. Numeral 115 refers to an oxide ion conducting electrolyte. Arrangements 100a and 100b include gas separator 130, which separates gaseous ammonia exhausted gases fed to separator 130 via passage 131. Numeral 140 marks electric energy provided by fuel cell 110 to a load (not shown). Anode area 113 is fluidly connected to separator 130 by passage 131. Anode area 113 is made of a cermet comprising transition metals such as Lanthanum, Cerium, Scandium, Titanium, Vanadium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Ruthenium, Rhodium, Palladium and Argentum. According to one embodiment of the present invention, anode area 113 is provided with a catalyst layer (not shown) made of made of a compound of transition metals and nitrogen {TM^oTM^ TM^ Ny where i and xi are positive integers Exhausting gases from cathode area 117 are vented to atmosphere. Feeding dry air to cathode area 117, generating gaseous ammonia therewithin and feeding the exhausting gases containing ammonia to separator 130 is also in the scope of the present invention. Electric energy generated by fuel cell 110 is designated by numeral 127. The heat generated in fuel cell 110 is transferred to separator 130 via passage 131.
Referring to Fig. 1 showing arrangement 100a, ammonia separated from exhausted gases is fed to ammonia tank 140 via passage 135. In Arrangement 100b (Fig. 2), separated ammonia is fed to
reformer 150 via passage 151. After reforming, obtained hydrogen and nitrogen are admixed via passages 153 and 155 to hydrogen or any hydrocarbon fuel fed to anode area 113 via passage 121.
Reference is now made Figs 3, 4 and 5 presenting alternative embodiments 200a, 200b and 200c of ammonia separators, respectively. Embodiment 150a in Fig. 3 includes ammonia absorber 270, ammonia evaporator 280 and dephlegmator 290. The exhausted gases are fed into ammonia absorber 270 via passage 131 based on absorbing ammonia from the exhausting gases in water. An ammonia solution obtained in absorber 270 then is fed into ammonia evaporator 280 via passage 275. Within evaporator 280, the aqueous ammonia solution is vaporized by the heat generated by fuel cell 110 (not shown) via heat transfer means 129. The vapor generated within ammonia evaporator 280 via passage 285 is provided to dephlegmator 290 where ammonia and water vapor fractions are separated. Separated ammonia outputs via passage 295.
Referring to Fig. 4 showing embodiment 200b, the exhausted gases via passage 131 are collected in tank 210 configured for storing exhausted tail gases. The exhausted gases stored in tank 210 are then pumped by compressor 220 via passages 215 and 225 and fed to membrane arrangement 260 configured for separating ammonia from the aforesaid exhausted gases. Separated ammonia (permeant gas) outputs from passage 265. Passage 265 is designed for venting retentate gases.
In Fig. 5, embodiment 200c is presented. The gases exhausted from the anode area (not shown) are fed to tank 210 via passage 131. Tank 230 is configured for accumulating the aforesaid exhausted gases. Then, the exhausted gases via passage 215 reach compressor 220 is used for pressurizing the exhausted gases. The pressurization of the exhausted gasses results in liquefying ammonia which is accumulated via passage 225 in tank 230 while other constituents of the pressurized gases are vented to the atmosphere via passage 235. Ammonia is cooled when it passes via expansion valve 240. Thereat, low-temperature gaseous ammonia can be used for cooling a working body circulating in loop 255 in heat-exchange arrangement 253. Finally, gaseous ammonia is provided via pipe 155 to a consumer.
Example 1::
Cathode: Eanthanum-Strontium Manganate/Cerium oxide doped with Gadolinium.
Electrolyte: Zirconium oxide stabilized by Scandium
Anode: Nickel oxide-Zirconium oxide stabilized by Scandium.
The fuel cell was fed with hydrogen and nitrogen (1:1 ratio) with flow rate of 0.4 1/min at the anode and air at the cathode with flow rate of 1 1/min. Operation temperature was about 800°C.
Example 2:
Cathode: Lanthanum-Strontium Manganate/Cerium oxide doped with Gadolinium.
Electrolyte: Zirconium oxide stabilized by Scandium and Cerium
Anode: Nickel-Zirconium oxide stabilized by Scandium provided with a layer of catalyst MmN. The catalyst layer is coated onto the anode by means of serigraphic deposition
The fuel cell was fed with hydrogen and nitrogen (1: 1 ratio) with flow rate 0.4 l/min at the anode and air at the cathode with flow rate of 1 1/min. Operation temperature was about 800°C. The results of characterization are in Table 1.
Although the invention has been described in conjunction with specific embodiments thereof, it is evident that many alternatives, modifications and variations will be apparent to those skilled in the art. Accordingly, it is intended to embrace all such alternatives, modifications and variations that fall within the spirit and broad scope of the appended claims.
Claims
1. A high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel and generating electricity and ammonia as a byproduct; said fuel cell comprising: a. a cathode area fed with air; b. an anode area fed with said fuel; and c. an oxide ion -conducting electrolyte area disposed between said cathode and anode areas; wherein said anode area is made of cermet comprising transition metals selected from the group consisting of Lanthanum, Cerium, Scandium, Titanium, Vanadium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Ruthenium, Rhodium, Palladium, Argentum and any combination thereof; said anode area when fed with a hydrogen-nitrogen mixture generates exhausted gases comprising gaseous ammonia.
2. The fuel cell arrangement according to claim 1 , wherein said anode area comprises a cermet Ni-ScSZ layer and a catalytic layer.
3. The fuel cell arrangement according to claim 1, wherein said catalytic layer comprises a compound of transition metals and nitrogen {TM^oTM^ TM^ Ny where i and xi are positive integers; said transition metals are selected from the group consisting of Lanthanum, Cerium, Scandium, Titanium, Vanadium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Ruthenium, Rhodium, Palladium, Argentum and any combination thereof.
4. The fuel cell arrangement according to claim 1 comprising a gas separator.
5. The fuel cell arrangement according to claim 4, wherein said gas separator comprises a compressor configured for pressurizing said exhausted gases.
6. The fuel cell arrangement according to claim 5, wherein said compressor is configured for pumping said exhausted gases via a membrane arrangement such that ammonia is separated from said exhausted gases.
7. The fuel cell arrangement according to claim 5, wherein said compressor configured for liquefying said gaseous ammonia while other constituents of the exhausted gases are vented to the atmosphere.
7
The fuel cell arrangement according to claim 4, wherein said gas separator comprises an ammonia absorber and an ammonia evaporator heated by heat generated by said fuel cell. A method of generating ammonia as a byproduct by a high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel; said method comprising steps of: a. providing a high-temperature solid oxide fuel cell arrangement fueled by a hydrogen or hydrocarbon fuel; said fuel cell comprising: i. a cathode area fed with air; ii. an anode area fed with said fuel-nitrogen mixture; and iii. an oxide ion -conducting electrolyte disposed between said cathode and anode areas; said anode area made of cermet comprising transition metals selected from the group consisting of Lanthanum, Cerium, Scandium, Titanium, Vanadium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Ruthenium, Rhodium, Palladium, Argentum and any combination thereof; b. feeding said fuel-nitrogen mixture to said anode area; c. fed air to said cathode area; d. operating said fuel cell; e. generating said ammonia as a byproduct in said anode area; and f. separating said ammonia from said exhausted stream.
8
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JP2011204416A (en) * | 2010-03-25 | 2011-10-13 | Nippon Shokubai Co Ltd | Fuel electrode material for solid oxide fuel battery, fuel electrode using the same, and cell for solid oxide fuel battery |
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US20190092645A1 (en) * | 2016-03-03 | 2019-03-28 | Jgc Corporation | Ammonia production method |
WO2020141500A1 (en) * | 2019-01-02 | 2020-07-09 | Ariel University Of Samaria | Solid oxide fuel cell arrangement generating ammonia as byproduct and utilizing ammonia as secondary fuel |
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US20120121999A1 (en) * | 2009-05-11 | 2012-05-17 | Commissariat A L'energie Atomique Et Aux Energies Alternatives | Cell of a high temperature fuel cell with internal reforming of hydrocarbons |
JP2011204416A (en) * | 2010-03-25 | 2011-10-13 | Nippon Shokubai Co Ltd | Fuel electrode material for solid oxide fuel battery, fuel electrode using the same, and cell for solid oxide fuel battery |
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