CA2586465A1 - Solid fuels for fuel cells - Google Patents
Solid fuels for fuel cells Download PDFInfo
- Publication number
- CA2586465A1 CA2586465A1 CA002586465A CA2586465A CA2586465A1 CA 2586465 A1 CA2586465 A1 CA 2586465A1 CA 002586465 A CA002586465 A CA 002586465A CA 2586465 A CA2586465 A CA 2586465A CA 2586465 A1 CA2586465 A1 CA 2586465A1
- Authority
- CA
- Canada
- Prior art keywords
- fuel
- metal
- solid
- mixtures
- oxygenate
- 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.)
- Abandoned
Links
- 239000000446 fuel Substances 0.000 title claims abstract description 145
- 239000004449 solid propellant Substances 0.000 title claims abstract description 41
- 239000000203 mixture Substances 0.000 claims abstract description 35
- 239000007787 solid Substances 0.000 claims abstract description 34
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 136
- 229910052751 metal Inorganic materials 0.000 claims description 29
- 239000002184 metal Substances 0.000 claims description 29
- 239000007800 oxidant agent Substances 0.000 claims description 19
- 239000011777 magnesium Substances 0.000 claims description 18
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 claims description 16
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims description 16
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 12
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims description 10
- 150000001875 compounds Chemical class 0.000 claims description 10
- 229910052749 magnesium Inorganic materials 0.000 claims description 9
- 239000000395 magnesium oxide Substances 0.000 claims description 9
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims description 9
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 claims description 9
- 150000004703 alkoxides Chemical class 0.000 claims description 7
- 229920001577 copolymer Polymers 0.000 claims description 7
- 229920000642 polymer Polymers 0.000 claims description 7
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 6
- 150000001342 alkaline earth metals Chemical class 0.000 claims description 6
- 239000011575 calcium Substances 0.000 claims description 6
- 239000004202 carbamide Substances 0.000 claims description 6
- 235000013877 carbamide Nutrition 0.000 claims description 6
- VTHJTEIRLNZDEV-UHFFFAOYSA-L magnesium dihydroxide Chemical compound [OH-].[OH-].[Mg+2] VTHJTEIRLNZDEV-UHFFFAOYSA-L 0.000 claims description 6
- 229910012375 magnesium hydride Inorganic materials 0.000 claims description 6
- 239000000347 magnesium hydroxide Substances 0.000 claims description 6
- 229910001862 magnesium hydroxide Inorganic materials 0.000 claims description 6
- 235000012254 magnesium hydroxide Nutrition 0.000 claims description 6
- 230000001590 oxidative effect Effects 0.000 claims description 6
- 150000001298 alcohols Chemical class 0.000 claims description 5
- VTIIJXUACCWYHX-UHFFFAOYSA-L disodium;carboxylatooxy carbonate Chemical compound [Na+].[Na+].[O-]C(=O)OOC([O-])=O VTIIJXUACCWYHX-UHFFFAOYSA-L 0.000 claims description 5
- 229910052744 lithium Inorganic materials 0.000 claims description 5
- 150000002736 metal compounds Chemical class 0.000 claims description 5
- 239000011734 sodium Substances 0.000 claims description 5
- 229940045872 sodium percarbonate Drugs 0.000 claims description 5
- 150000001299 aldehydes Chemical class 0.000 claims description 4
- CRGZYKWWYNQGEC-UHFFFAOYSA-N magnesium;methanolate Chemical compound [Mg+2].[O-]C.[O-]C CRGZYKWWYNQGEC-UHFFFAOYSA-N 0.000 claims description 4
- 150000001451 organic peroxides Chemical class 0.000 claims description 4
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 claims description 3
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 claims description 3
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 claims description 3
- 229910052788 barium Inorganic materials 0.000 claims description 3
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 claims description 3
- 229910052791 calcium Inorganic materials 0.000 claims description 3
- -1 carbonyl vinyl Chemical group 0.000 claims description 3
- 150000002148 esters Chemical class 0.000 claims description 3
- 150000002170 ethers Chemical class 0.000 claims description 3
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims description 3
- 150000007524 organic acids Chemical class 0.000 claims description 3
- 235000005985 organic acids Nutrition 0.000 claims description 3
- 229920000058 polyacrylate Polymers 0.000 claims description 3
- 229910052700 potassium Inorganic materials 0.000 claims description 3
- 239000011591 potassium Substances 0.000 claims description 3
- 229910052708 sodium Inorganic materials 0.000 claims description 3
- 229910052712 strontium Inorganic materials 0.000 claims description 3
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 claims description 3
- 235000000346 sugar Nutrition 0.000 claims description 3
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 claims description 2
- NIXOWILDQLNWCW-UHFFFAOYSA-N 2-Propenoic acid Natural products OC(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 claims description 2
- HRPVXLWXLXDGHG-UHFFFAOYSA-N Acrylamide Chemical compound NC(=O)C=C HRPVXLWXLXDGHG-UHFFFAOYSA-N 0.000 claims description 2
- 239000004716 Ethylene/acrylic acid copolymer Substances 0.000 claims description 2
- 229920002125 Sokalan® Polymers 0.000 claims description 2
- IKHGUXGNUITLKF-XPULMUKRSA-N acetaldehyde Chemical compound [14CH]([14CH3])=O IKHGUXGNUITLKF-XPULMUKRSA-N 0.000 claims description 2
- 229910052783 alkali metal Inorganic materials 0.000 claims description 2
- 150000001340 alkali metals Chemical class 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
- 150000001412 amines Chemical class 0.000 claims description 2
- 229910052790 beryllium Inorganic materials 0.000 claims description 2
- ATBAMAFKBVZNFJ-UHFFFAOYSA-N beryllium atom Chemical compound [Be] ATBAMAFKBVZNFJ-UHFFFAOYSA-N 0.000 claims description 2
- 229910052792 caesium Inorganic materials 0.000 claims description 2
- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical compound [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 claims description 2
- 150000004649 carbonic acid derivatives Chemical class 0.000 claims description 2
- 125000005594 diketone group Chemical group 0.000 claims description 2
- 150000002009 diols Chemical class 0.000 claims description 2
- 239000003995 emulsifying agent Substances 0.000 claims description 2
- 150000002576 ketones Chemical class 0.000 claims description 2
- 150000003891 oxalate salts Chemical class 0.000 claims description 2
- 229920005862 polyol Polymers 0.000 claims description 2
- 150000003077 polyols Chemical class 0.000 claims description 2
- 229910052701 rubidium Inorganic materials 0.000 claims description 2
- IGLNJRXAVVLDKE-UHFFFAOYSA-N rubidium atom Chemical compound [Rb] IGLNJRXAVVLDKE-UHFFFAOYSA-N 0.000 claims description 2
- 150000008163 sugars Chemical class 0.000 claims description 2
- 150000004072 triols Chemical class 0.000 claims description 2
- 229920002554 vinyl polymer Polymers 0.000 claims description 2
- 229910052723 transition metal Inorganic materials 0.000 claims 2
- 150000003624 transition metals Chemical class 0.000 claims 2
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 claims 1
- 239000011949 solid catalyst Substances 0.000 claims 1
- 239000007788 liquid Substances 0.000 abstract description 19
- 239000000376 reactant Substances 0.000 abstract description 3
- 210000004027 cell Anatomy 0.000 description 61
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 30
- 229910002092 carbon dioxide Inorganic materials 0.000 description 17
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 16
- 239000001569 carbon dioxide Substances 0.000 description 15
- 238000006243 chemical reaction Methods 0.000 description 13
- 239000001257 hydrogen Substances 0.000 description 13
- 229910052739 hydrogen Inorganic materials 0.000 description 13
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 12
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 10
- JILPJDVXYVTZDQ-UHFFFAOYSA-N lithium methoxide Chemical compound [Li+].[O-]C JILPJDVXYVTZDQ-UHFFFAOYSA-N 0.000 description 10
- 239000000126 substance Substances 0.000 description 10
- 239000002912 waste gas Substances 0.000 description 9
- IKHGUXGNUITLKF-UHFFFAOYSA-N Acetaldehyde Chemical compound CC=O IKHGUXGNUITLKF-UHFFFAOYSA-N 0.000 description 8
- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 description 8
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 7
- 239000003513 alkali Substances 0.000 description 7
- 229940077744 antacid containing magnesium compound Drugs 0.000 description 7
- 150000002681 magnesium compounds Chemical class 0.000 description 7
- 239000000463 material Substances 0.000 description 7
- 239000003054 catalyst Substances 0.000 description 6
- 229910000000 metal hydroxide Inorganic materials 0.000 description 6
- 150000004692 metal hydroxides Chemical class 0.000 description 6
- 150000002739 metals Chemical class 0.000 description 6
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 5
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 5
- 230000006872 improvement Effects 0.000 description 5
- 150000002978 peroxides Chemical class 0.000 description 5
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 5
- 238000012360 testing method Methods 0.000 description 5
- 239000012808 vapor phase Substances 0.000 description 5
- JVTIXNMXDLQEJE-UHFFFAOYSA-N 2-decanoyloxypropyl decanoate 2-octanoyloxypropyl octanoate Chemical compound C(CCCCCCC)(=O)OCC(C)OC(CCCCCCC)=O.C(=O)(CCCCCCCCC)OCC(C)OC(=O)CCCCCCCCC JVTIXNMXDLQEJE-UHFFFAOYSA-N 0.000 description 4
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 4
- 229940075510 carbopol 981 Drugs 0.000 description 4
- 238000000354 decomposition reaction Methods 0.000 description 4
- 238000011161 development Methods 0.000 description 4
- 239000007791 liquid phase Substances 0.000 description 4
- 239000012528 membrane Substances 0.000 description 4
- 229910052987 metal hydride Inorganic materials 0.000 description 4
- 150000004681 metal hydrides Chemical class 0.000 description 4
- 238000000034 method Methods 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- 238000002407 reforming Methods 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- CIHOLLKRGTVIJN-UHFFFAOYSA-N tert‐butyl hydroperoxide Chemical compound CC(C)(C)OO CIHOLLKRGTVIJN-UHFFFAOYSA-N 0.000 description 4
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 3
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 3
- 208000021017 Weight Gain Diseases 0.000 description 3
- 229910017052 cobalt Inorganic materials 0.000 description 3
- 239000010941 cobalt Substances 0.000 description 3
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 3
- 239000010949 copper Substances 0.000 description 3
- 230000005611 electricity Effects 0.000 description 3
- 239000012530 fluid Substances 0.000 description 3
- 239000010931 gold Substances 0.000 description 3
- 150000002430 hydrocarbons Chemical class 0.000 description 3
- 239000011572 manganese Substances 0.000 description 3
- 238000002844 melting Methods 0.000 description 3
- 230000008018 melting Effects 0.000 description 3
- 229910044991 metal oxide Inorganic materials 0.000 description 3
- 150000004706 metal oxides Chemical class 0.000 description 3
- 229910052759 nickel Inorganic materials 0.000 description 3
- 238000010248 power generation Methods 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- 239000010948 rhodium Substances 0.000 description 3
- 230000004584 weight gain Effects 0.000 description 3
- 239000004343 Calcium peroxide Substances 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- SPAGIJMPHSUYSE-UHFFFAOYSA-N Magnesium peroxide Chemical compound [Mg+2].[O-][O-] SPAGIJMPHSUYSE-UHFFFAOYSA-N 0.000 description 2
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-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
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 2
- LHJQIRIGXXHNLA-UHFFFAOYSA-N calcium peroxide Chemical compound [Ca+2].[O-][O-] LHJQIRIGXXHNLA-UHFFFAOYSA-N 0.000 description 2
- 235000019402 calcium peroxide Nutrition 0.000 description 2
- 229910002091 carbon monoxide Inorganic materials 0.000 description 2
- 239000011651 chromium Substances 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 2
- 229910052737 gold Inorganic materials 0.000 description 2
- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 2
- 229910052741 iridium Inorganic materials 0.000 description 2
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 2
- 229910052742 iron Inorganic materials 0.000 description 2
- 150000002642 lithium compounds Chemical class 0.000 description 2
- 238000011068 loading method Methods 0.000 description 2
- 229960004995 magnesium peroxide Drugs 0.000 description 2
- 229910052748 manganese Inorganic materials 0.000 description 2
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 2
- 229910052750 molybdenum Inorganic materials 0.000 description 2
- 239000011733 molybdenum Substances 0.000 description 2
- 239000010955 niobium Substances 0.000 description 2
- 150000002894 organic compounds Chemical class 0.000 description 2
- 229910052762 osmium Inorganic materials 0.000 description 2
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 description 2
- 229910052763 palladium Inorganic materials 0.000 description 2
- 239000012071 phase Substances 0.000 description 2
- 229910052697 platinum Inorganic materials 0.000 description 2
- 230000000379 polymerizing effect Effects 0.000 description 2
- 229910052702 rhenium Inorganic materials 0.000 description 2
- WUAPFZMCVAUBPE-UHFFFAOYSA-N rhenium atom Chemical compound [Re] WUAPFZMCVAUBPE-UHFFFAOYSA-N 0.000 description 2
- 229910052703 rhodium Inorganic materials 0.000 description 2
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 2
- 229910052707 ruthenium Inorganic materials 0.000 description 2
- 229910052709 silver Inorganic materials 0.000 description 2
- 239000004332 silver Substances 0.000 description 2
- 239000012265 solid product Substances 0.000 description 2
- 239000010936 titanium Substances 0.000 description 2
- 238000009834 vaporization Methods 0.000 description 2
- 230000008016 vaporization Effects 0.000 description 2
- 235000019786 weight gain Nutrition 0.000 description 2
- 230000004580 weight loss Effects 0.000 description 2
- XRXANEMIFVRKLN-UHFFFAOYSA-N 2-hydroperoxy-2-methylbutane Chemical compound CCC(C)(C)OO XRXANEMIFVRKLN-UHFFFAOYSA-N 0.000 description 1
- ODINCKMPIJJUCX-UHFFFAOYSA-N Calcium oxide Chemical compound [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 description 1
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- KEAYESYHFKHZAL-UHFFFAOYSA-N Sodium Chemical compound [Na] KEAYESYHFKHZAL-UHFFFAOYSA-N 0.000 description 1
- HVUMOYIDDBPOLL-XWVZOOPGSA-N Sorbitan monostearate Chemical compound CCCCCCCCCCCCCCCCCC(=O)OC[C@@H](O)[C@H]1OC[C@H](O)[C@H]1O HVUMOYIDDBPOLL-XWVZOOPGSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- 230000003213 activating effect Effects 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 150000004974 alkaline earth metal peroxides Chemical class 0.000 description 1
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical compound [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 210000000170 cell membrane Anatomy 0.000 description 1
- 210000003850 cellular structure Anatomy 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 230000003750 conditioning effect Effects 0.000 description 1
- 238000011109 contamination Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- ZFTFAPZRGNKQPU-UHFFFAOYSA-N dicarbonic acid Chemical class OC(=O)OC(O)=O ZFTFAPZRGNKQPU-UHFFFAOYSA-N 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 239000012895 dilution Substances 0.000 description 1
- 238000010790 dilution Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000007792 gaseous phase Substances 0.000 description 1
- 150000002334 glycols Chemical class 0.000 description 1
- 229910052735 hafnium Inorganic materials 0.000 description 1
- VBJZVLUMGGDVMO-UHFFFAOYSA-N hafnium atom Chemical compound [Hf] VBJZVLUMGGDVMO-UHFFFAOYSA-N 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- XGZVUEUWXADBQD-UHFFFAOYSA-L lithium carbonate Chemical compound [Li+].[Li+].[O-]C([O-])=O XGZVUEUWXADBQD-UHFFFAOYSA-L 0.000 description 1
- 229910052808 lithium carbonate Inorganic materials 0.000 description 1
- 229910000103 lithium hydride Inorganic materials 0.000 description 1
- 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 description 1
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
- 229910052753 mercury Inorganic materials 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Natural products C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 150000004704 methoxides Chemical class 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 230000003071 parasitic effect Effects 0.000 description 1
- 239000012466 permeate Substances 0.000 description 1
- NTTOTNSKUYCDAV-UHFFFAOYSA-N potassium hydride Chemical compound [KH] NTTOTNSKUYCDAV-UHFFFAOYSA-N 0.000 description 1
- 229910000105 potassium hydride Inorganic materials 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 229910052706 scandium Inorganic materials 0.000 description 1
- SIXSYDAISGFNSX-UHFFFAOYSA-N scandium atom Chemical compound [Sc] SIXSYDAISGFNSX-UHFFFAOYSA-N 0.000 description 1
- VSZWPYCFIRKVQL-UHFFFAOYSA-N selanylidenegallium;selenium Chemical compound [Se].[Se]=[Ga].[Se]=[Ga] VSZWPYCFIRKVQL-UHFFFAOYSA-N 0.000 description 1
- 229910000104 sodium hydride Inorganic materials 0.000 description 1
- 239000012312 sodium hydride Substances 0.000 description 1
- 239000007790 solid phase Substances 0.000 description 1
- 239000002910 solid waste Substances 0.000 description 1
- 239000001587 sorbitan monostearate Substances 0.000 description 1
- 229940035048 sorbitan monostearate Drugs 0.000 description 1
- 235000011076 sorbitan monostearate Nutrition 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 150000003464 sulfur compounds Chemical class 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- 229910052713 technetium Inorganic materials 0.000 description 1
- GKLVYJBZJHMRIY-UHFFFAOYSA-N technetium atom Chemical compound [Tc] GKLVYJBZJHMRIY-UHFFFAOYSA-N 0.000 description 1
- JBQYATWDVHIOAR-UHFFFAOYSA-N tellanylidenegermanium Chemical compound [Te]=[Ge] JBQYATWDVHIOAR-UHFFFAOYSA-N 0.000 description 1
- 150000003568 thioethers Chemical class 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- 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
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C31/00—Saturated compounds having hydroxy or O-metal groups bound to acyclic carbon atoms
- C07C31/28—Metal alcoholates
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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
- H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
- H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
- H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material
- H01M8/0643—Gasification of solid fuel
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/12—Feeding the process for making hydrogen or synthesis gas
- C01B2203/1205—Composition of the feed
- C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
- C01B2203/1217—Alcohols
- C01B2203/1223—Methanol
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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
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/12—Feeding the process for making hydrogen or synthesis gas
- C01B2203/1258—Pre-treatment of the feed
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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
- H01M8/04—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
- H01M8/04201—Reactant storage and supply, e.g. means for feeding, pipes
- H01M8/04208—Cartridges, cryogenic media or cryogenic reservoirs
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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
- H01M8/04—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
- H01M8/04201—Reactant storage and supply, e.g. means for feeding, pipes
- H01M8/04216—Reactant storage and supply, e.g. means for feeding, pipes characterised by the choice for a specific material, e.g. carbon, hydride, absorbent
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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
- H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
- H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
- H01M8/065—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants by dissolution of metals or alloys; by dehydriding metallic substances
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- 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
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- 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
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- Y02E60/50—Fuel cells
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Abstract
A solid fuel for use in fuel cells. The solid fuel includes solid oxygenates, and mixtures for generating a gaseous fuel from the solid fuel. The solid fuel can be contained in a cartridge and reacted with a liquid reactant for generating a gaseous fuel used in the fuel cell.
Description
SOLID FUELS FOR FUEL CELLS
BACKGROUND OF THE INVENTION
[0001] Fuel cells have developed as a method of generating electricity from chemicals.
Some early development focused on using hydrogen as a clean fuel source for producing power. Work has been done on the storage and generation of hydrogen for use in fuel cells and is disclosed in US 6,057,051, US 6,267,229, US 6,251,349, US 6,459,231, and US
6,514,478.
Hydrogen is a high energy, low pollution fuel, however, the storage of this fuel is cumbersome, both from an energy density and safety point of view.
BACKGROUND OF THE INVENTION
[0001] Fuel cells have developed as a method of generating electricity from chemicals.
Some early development focused on using hydrogen as a clean fuel source for producing power. Work has been done on the storage and generation of hydrogen for use in fuel cells and is disclosed in US 6,057,051, US 6,267,229, US 6,251,349, US 6,459,231, and US
6,514,478.
Hydrogen is a high energy, low pollution fuel, however, the storage of this fuel is cumbersome, both from an energy density and safety point of view.
[0002] The difficulty of storing hydrogen has led to looking at the generation of hydrogen from more useful fuels. Liquid fuels containing a relatively high amount of hydrogen that can be generated through reforming have received significant attention. Reforming of a fuel is expensive, and adds significantly to the complexity and size of a unit using fuel cells for power generation. Reformers and methods of reforming liquid fuels have been developed, as shown in US 4,716,859, US 6,238,815, and US 6,277,330. Therefore, there is significant interest in fuel cells that can use a hydrogen rich fuel that can be processed directly over a fuel cell electrode. This separates the fuel cells into two general categories: an indirect or reformer fuel cell wherein a fuel, usually an organic fuel, is reformed and processed to produce a hydrogen rich, and substantially carbon monoxide (CO) free feed stream to the fuel cell; and a direct oxidation fuel cell wherein an organic fuel is directly fed to the fuel cell and oxidized without any chemical reforming. Direct oxidation fuel cells can use either a liquid feed design or a vapor feed design, and preferably the fuels, after oxidation in the fuel cell, yield clean combustion products like water and carbon dioxide (CO2).
[0003] In early development of direct methanol fuel cells (DMFC), using gaseous methanol required a high heat, which brought about the degradation of the fuel cell membranes. This led to the development of DMFCs using methanol in the liquid phase, as shown in US 5,599,638, and US 6,248,460. However, the liquid phase presents drawbacks also, not the least of which is cross over of the membrane by the methanol and contamination of the cathode.
[0004] As with vapor phase fuel cells, liquid phase fuel cells also have handling problems.
Specific problems include the orientation of the fuel cells or portable devices such that liquid fuel can flow out of openings for releasing waste gases, and liquid fuel cells have the problem of the high concentration of liquid methanol permeating through to be oxidized at the cathode which reduces fuel cell efficiency.
SUMMARY OF THE INVENTION
Specific problems include the orientation of the fuel cells or portable devices such that liquid fuel can flow out of openings for releasing waste gases, and liquid fuel cells have the problem of the high concentration of liquid methanol permeating through to be oxidized at the cathode which reduces fuel cell efficiency.
SUMMARY OF THE INVENTION
[0005] The present invention is a solid fuel for use in a fuel cell. The solid fuel comprises a solid oxygenate that is selected from metal oxygenates, gelled oxygenates, and frozen oxygenates. The invention particularly includes as a solid fuel a mixture of an oxygenate, such as methanol or acetaldehyde, and a polymer, such as an acrylic polymer in amounts necessary to produce a solid gel.
[0006] In one embodiment, the invention comprises the addition of a metal or metal compound wherein the metal is selected from the group consisting of alkali metals, alkaline earth metals, and mixtures thereof. In particular, the preferred metal compounds include magnesium compounds such as magnesium hydroxide, magnesium oxide, magnesium methoxide, magnesium hydride, and mixtures thereof. A preferred metal is magnesium. The metal compounds enhance the behavior of the oxygenates, and provide for a material to adsorb carbon dioxide generated at the anode.
[0007] In another embodiment, the invention comprises the addition of an oxidizing agent.
The oxidizing agent is selected from the group consisting of sodium percarbonate, carbamide liydrogen peroxide, organic peroxides, calcium peroxide, magnesium peroxide, and mixtures thereof. The addition of oxidizing agents enhances the power density of the fuel in a direct methanol fuel cell.
The oxidizing agent is selected from the group consisting of sodium percarbonate, carbamide liydrogen peroxide, organic peroxides, calcium peroxide, magnesium peroxide, and mixtures thereof. The addition of oxidizing agents enhances the power density of the fuel in a direct methanol fuel cell.
[0008] Other objects, advantages and applications of the present invention will become apparent to those skilled in the art from the following detailed description.
BRIEF DESCRIPTION OF THE FIGURES
BRIEF DESCRIPTION OF THE FIGURES
[0009] Figure 1 shows the stability of several chemical compounds and mixtures;
[0010] Figure 2 shows a comparison of DMFC liquid and solid fuel;
[0011] Figures 3 and 4 show comparisons of current against cell potential for different compositions of solid fuels and liquid methanol;
[0012] Figures 5 and 6 show comparisons of current against cell potential for different compositions of solid fuels;
[0013] Figure 7 shows a comparison of solid acetaldehyde fuel and solid methanol fuel;
[0014] Figure 8 shows the effect of additional oxidant added to methanol for a direct methanol fuel cell;
[0015] Figure 9 shows the I-V (current-voltage) curves for different hydrogen peroxide with methanol for a direct methanol fuel cell;
[0016] Figure 10 shows the voltage and amperage for a fuel cell with magnesium and solid methanol with a pulse of sulfuric acid;
[0017] Figure 11 shows the voltage, amperage and power density for magnesium and solid methanol in a fuel cell with a pulse of sulfuric acid; and [0018] Figure 12 shows the power density and the pressure for magnesium and solid methanol in a fuel cell with a pulse of sulfuric acid.
DETAILED DESCRIPTION OF THE INVENTION
DETAILED DESCRIPTION OF THE INVENTION
[0019] The present invention comprises a new fuel for use in a fuel cell. The new fuels are solid fuels and are not restricted to the type of fuel cells they can be used in, and can include proton exchange membrane (PEM) fuel cells, solid oxide fuel cells (SOFC), phosphoric acid fuel cells (PAFC), direct methanol fuel cells (DMFC), molten carbonate fuel cells (MCFC), and alkaline fuel cells (AFC).
[0020] To overcome drawbacks to liquid fuel cells, alternate methods of handling a liquid fuel have been developed. These include binding the liquid fuel in a non-fluid state, wherein when the fuel is needed, the fuel is recovered in a fluid state, as presented in US 4,493,878.
This still has the drawbacks of a liquid fuel in that the cathode efficiency is reduced from the permeation of the liquid fuel through the anode. Methanol crossover through the membrane causes a partial shorting of the cell, leading to a lower potential. Membrane development to mitigate this diffusion process is ongoing. In the meantime, concentrations of methanol are typically limited to 1-2 moles/1, i.e. 7 wt%. This results in a quick fall off in the current-voltage (I-V) curve, significant parasitic power loss for pump arounds, and a relatively large amount of processing steps and fuel cell components for anode feed conditioning.
This still has the drawbacks of a liquid fuel in that the cathode efficiency is reduced from the permeation of the liquid fuel through the anode. Methanol crossover through the membrane causes a partial shorting of the cell, leading to a lower potential. Membrane development to mitigate this diffusion process is ongoing. In the meantime, concentrations of methanol are typically limited to 1-2 moles/1, i.e. 7 wt%. This results in a quick fall off in the current-voltage (I-V) curve, significant parasitic power loss for pump arounds, and a relatively large amount of processing steps and fuel cell components for anode feed conditioning.
[0021] What is needed is a fuel that is easier to handle and readily generates a gaseous component for use in a fuel cell. The solid fuel provides greater energy density and ease of handling. A solid fuel allows for convenient loading, removal, and replacement into a fuel cell. A solid fuel reduces risk of leaks and spills, as can occur with liquid or gaseous fuels.
And a solid fuel allows for lighter containers than would be available for gaseous fuels. In addition, as a solid, the orientation of the fuel cell is irrelevant, as the fuel after loading into a fuel cell does not move independently, and will maintain a fixed position relative to the anode.
The fuel can be any solid chemical that generates an appropriate fuel, such as an oxygenate or hydrogen for direct oxidation at the fuel cell anode. The fuel is comprised of a mixture of fuel components, and the fuel components are any chemical compounds that are added to the fuel mixture. An oxygenate is a hydrocarbon compound that has been altered with the addition of at least one oxygen atom to the hydrocarbon compound. Oxygenates include, but are not limited to, alcohols, diols, triols, aldehydes, ethers, ketones, diketones, esters, carbonates, dicarbonates, oxalates, organic acids, sugars, and mixtures thereof. Upon reaction of the solid oxygenate, a gaseous oxygenate such as methanol is produced for reaction in the fuel cell.
And a solid fuel allows for lighter containers than would be available for gaseous fuels. In addition, as a solid, the orientation of the fuel cell is irrelevant, as the fuel after loading into a fuel cell does not move independently, and will maintain a fixed position relative to the anode.
The fuel can be any solid chemical that generates an appropriate fuel, such as an oxygenate or hydrogen for direct oxidation at the fuel cell anode. The fuel is comprised of a mixture of fuel components, and the fuel components are any chemical compounds that are added to the fuel mixture. An oxygenate is a hydrocarbon compound that has been altered with the addition of at least one oxygen atom to the hydrocarbon compound. Oxygenates include, but are not limited to, alcohols, diols, triols, aldehydes, ethers, ketones, diketones, esters, carbonates, dicarbonates, oxalates, organic acids, sugars, and mixtures thereof. Upon reaction of the solid oxygenate, a gaseous oxygenate such as methanol is produced for reaction in the fuel cell.
[0022] One preferred group of oxygenates is metal alkoxides, that react with water to generate an oxygenate in a vapor phase for reaction at the anode of the fuel cell. By generating the oxygenate in the gas phase, the fuel overcomes limitations due to the liquid phase fuel cells wherein the liquid fuel overloads the fuel cell and permeates through to the cathode. Preferred metal oxygenates include metal alkoxides. Appropriate metals include, but are not limited to, alkali and alkaline earth metals, and are selected from lithium (Li), sodium (Na), potassium (K), beryllium (Be), magnesium (Mg), and calcium (Ca). Other appropriate metals include rubidium (Rb), cesium (Cs), strontium (Sr), barium (Ba), and aluminum (Al).
The oxygenate produced for use in the fuel cell preferably has a boiling point of less than 100 C. Preferably oxygenates include low molecular weight alcohols, aldehydes, organic acids, and ethers.
The oxygenate produced for use in the fuel cell preferably has a boiling point of less than 100 C. Preferably oxygenates include low molecular weight alcohols, aldehydes, organic acids, and ethers.
[0023] Alkali alkoxides, and in particular alkali methoxides and ethoxides, are very reactive and pyrophoric materials. Adding water produces a vigorous reaction and heat sufficient to vaporize the alcohol generated from the reaction.
[0024] A particular alkoxide studied was lithium methoxide (LiOCH3). Lithium methoxide reacts with water to generate lithium hydroxide and methanol, with sufficient heat to generate the methanol in the vapor phase, as shown in equation 1.
LiOCH3(s) + HaO(g) 4 LiOH(s) + HOCH3(g) eqn. 1.
LiOCH3(s) + HaO(g) 4 LiOH(s) + HOCH3(g) eqn. 1.
[0025] The stability of lithium methoxide was studied, along with the stability of several oxidants. The experiment was carried out at room temperature in air saturated with water.
Samples were weighed over time. It was found that the samples underwent a weight loss and subsequent weight gain, with the results shown in Figure 1. Without being bound to a particular theory, it is believed that the solid fuel (lithium methoxide) reacts with the water vapor generating methanol and subsequently lose weight. The subsequent weight gain is due to the reaction of the lithium hydroxide with carbon dioxide in the air forming a carbonate, as in equation 2.
2LiOH(s) + C02(g) 4 Li2CO3(s) + H20 eqn. 2.
Samples were weighed over time. It was found that the samples underwent a weight loss and subsequent weight gain, with the results shown in Figure 1. Without being bound to a particular theory, it is believed that the solid fuel (lithium methoxide) reacts with the water vapor generating methanol and subsequently lose weight. The subsequent weight gain is due to the reaction of the lithium hydroxide with carbon dioxide in the air forming a carbonate, as in equation 2.
2LiOH(s) + C02(g) 4 Li2CO3(s) + H20 eqn. 2.
[0026] The fuel should be sealed in a container that is moisture impermeable to prevent consumption of the fuel through exposure to the atmosphere. The fuel container is opened when in use, but sealed against the anode forming a compartment closed to the atmosphere.
This is to prevent loss of fuel, as well as to prevent excess moisture affecting the fuel. The fuel consumption is therefore controlled by moisture allowed into the compartm.ent.
This is to prevent loss of fuel, as well as to prevent excess moisture affecting the fuel. The fuel consumption is therefore controlled by moisture allowed into the compartm.ent.
[0027] Additional compositions were studied, showing similar results in weight losses and gains in Figure 1, and are listed in Table 1. Some of the test fuels included a small amount of catalyst, Mn02, to facilitate the decomposition of an exothermic reactant. The exothennic reactant generates heat to vaporize the fuel.
Table 1 Solid Fuel 1 Lithium Methoxide (LiOCH3) Solid Fuel 2 LiOCH3+ Sodium percarbonate + Mn02 Solid Fue13 Sodium Percarbonate + Mn02 Solid Fuel 4 LiOCH3 + Carbamide*H202 + Mn02 Solid Fuel 5 Carbamide*H202 + Mn02 [0028] This leads to the further theory of using a solid fuel to be activated by exposure to water, including in the vapor phase, generating fuel and heat and subsequently absorbing waste gases to form a solid phase. Other activation means include, but are not limited to the application of heat, application of electrical current and exposure to carbon dioxide. As the fuel reacts at the anode, waste gases are generated. For example, methanol reacts at the anode and generates carbon dioxide and water in addition to the electricity generated during the reaction, according to equation 3.
CH3OH + 1.502 -> 2Ha0 + CO2 + electricity eqn. 3.
Table 1 Solid Fuel 1 Lithium Methoxide (LiOCH3) Solid Fuel 2 LiOCH3+ Sodium percarbonate + Mn02 Solid Fue13 Sodium Percarbonate + Mn02 Solid Fuel 4 LiOCH3 + Carbamide*H202 + Mn02 Solid Fuel 5 Carbamide*H202 + Mn02 [0028] This leads to the further theory of using a solid fuel to be activated by exposure to water, including in the vapor phase, generating fuel and heat and subsequently absorbing waste gases to form a solid phase. Other activation means include, but are not limited to the application of heat, application of electrical current and exposure to carbon dioxide. As the fuel reacts at the anode, waste gases are generated. For example, methanol reacts at the anode and generates carbon dioxide and water in addition to the electricity generated during the reaction, according to equation 3.
CH3OH + 1.502 -> 2Ha0 + CO2 + electricity eqn. 3.
[0029] The carbon dioxide is a waste gas that must be disposed of in some manner. With the present invention, the carbon dioxide reacts with the fuel waste product, such as a metal hydroxide, and forms a solid. A preferred fuel will contain components that absorb, or react with the waste gases from the fuel cell. Fuel components may include but are not limited to, metal oxides and metal hydroxides. The waste gases are reacted to form a solid product, or are absorbed onto a solid. The primary waste gases for a direct methanol fuel cell are carbon dioxide and water. The water will react with the fuel to form more oxygenate in the vapor phase. When the fuel is metal alkoxide, where the metal is an alkali or alkaline earth metal, the metal will form a hydroxide reacting with water to give up the alcohol. The metal hydroxide will subsequently react with the carbon dioxide generated at the anode and remove the carbon dioxide from the gas phase to form a carbonate solid product.
[0030] Other preferred fuels included gelled oxygenates and frozen oxygenates.
The gelled oxygenates are oxygenates that have a polymer added to form a solid.
One example of a gelled oxygenate comprises a mixture of 5 wt. % of CarbopolTm 981 polymer and 95 wt. % of methanol. Carbopol 981 is an acrylic polymer made by B.F. Goodrich of Akron, Ohio. The gelled oxygenate when heated releases the methanol, which is vaporized and available for use at the anode. The oxygenate in the solid fuel comprises at least 30% by weight of the fuel, and preferably at least 50% by weight. For gelled or frozen oxygenates, the fuel comprises additional compounds for absorbing waste gases from the anode. Additional fuel components for gelled and frozen oxygenates include metals, metal oxides, metal hydroxides, or metal hydrides. Preferably the metals, metal oxides, metal hydroxides, and metal hydrides comprise alkali or alkaline earth metals. The additional components provide heat to vaporize the oxygenates and provide components for removing anode waste gases through absorption or reaction to form solid waste products.
The gelled oxygenates are oxygenates that have a polymer added to form a solid.
One example of a gelled oxygenate comprises a mixture of 5 wt. % of CarbopolTm 981 polymer and 95 wt. % of methanol. Carbopol 981 is an acrylic polymer made by B.F. Goodrich of Akron, Ohio. The gelled oxygenate when heated releases the methanol, which is vaporized and available for use at the anode. The oxygenate in the solid fuel comprises at least 30% by weight of the fuel, and preferably at least 50% by weight. For gelled or frozen oxygenates, the fuel comprises additional compounds for absorbing waste gases from the anode. Additional fuel components for gelled and frozen oxygenates include metals, metal oxides, metal hydroxides, or metal hydrides. Preferably the metals, metal oxides, metal hydroxides, and metal hydrides comprise alkali or alkaline earth metals. The additional components provide heat to vaporize the oxygenates and provide components for removing anode waste gases through absorption or reaction to form solid waste products.
[0031] Additional materials added to the solid oxygenates include hydroreactive materials for generating heat upon the addition of water. Preferably the materials contribute additional fuel, such as hydrogen, and/or peroxide for adsorption of carbon dioxide.
Preferred materials include metal hydrides, such as lithium hydride, magnesium hydride, sodium hydride, potassium hydride, aluminum hydride, and mixtures thereof.
Preferred materials include metal hydrides, such as lithium hydride, magnesium hydride, sodium hydride, potassium hydride, aluminum hydride, and mixtures thereof.
[0032] Solid fuels can be formed by using selected chemicals to polymerize an organic solution to gel the organic compound. The polymerizing chemicals comprise at least 3% by weight of the solid fuel. Chemicals for forming the gel include, but are not limited to, acrylic acid/acrylic amide based polymers, copolymers of polyols, ethylene/acrylic acid copolymers with amine emulsifiers, carboxyl vinyl polymers, polyacrylic acid polymers, olefin-maleic anhydride copolymers, and copolymers of oligomers containing OH groups with formaldehyde. The copolymers of oligomers containing OH groups include high melting point alcohols, i.e. alcohols having 12 or more carbons; high melting point glycols;
high melting point hydrocarbons; sugar esters, i.e., Sorbitan Monostearate (S-MAZ 60); and alkali alkoxides. Additional polymerizing materials can be found in US 3,759,674; US
3,148,958;
US 3,214,252; US 4,261,700; and US 4,865,971.
high melting point hydrocarbons; sugar esters, i.e., Sorbitan Monostearate (S-MAZ 60); and alkali alkoxides. Additional polymerizing materials can be found in US 3,759,674; US
3,148,958;
US 3,214,252; US 4,261,700; and US 4,865,971.
[0033] A study of a particular gelled fuel was done to demonstrate the use of a gelled fuel.
The fuel comprised methanol, calcium oxide (CaO), and Carbopol 981 polymer with a ratio of 32:56:5 respectively. The fuel was loaded into a DMFC and the fuel cell was run. The fuel cell generated an I-V curve for comparison with an aqueous methanol fuel at different temperatures, and at ambient pressure. Figure 2 shows the results of the I-V
curve for comparison with a liquid fuel.
The fuel comprised methanol, calcium oxide (CaO), and Carbopol 981 polymer with a ratio of 32:56:5 respectively. The fuel was loaded into a DMFC and the fuel cell was run. The fuel cell generated an I-V curve for comparison with an aqueous methanol fuel at different temperatures, and at ambient pressure. Figure 2 shows the results of the I-V
curve for comparison with a liquid fuel.
[0034] The composition of fuel can be adjusted to compensate for additional water generated or absorbed by the fuel, and additional heat necessary to ensure vaporization of the fuel when exposed to moisture. Additional heat can be generated by using chemicals that have very exothermic reactions upon addition of water or an appropriate chemical that generates heat upon decomposition. Examples of appropriate chemicals include, but are not limited to, organic peroxides, and carbamide hydrogen peroxide. The fuel composition can also be adjusted by using a combination of the above mentioned fuels, for example, mixing a metal hydride with a metal oxygenate to form a fuel that will generate hydrogen and an alcohol for reaction at the fuel cell anode. Alternate mixtures might include additional metal hydroxides for more rapid reaction of carbon dioxide generated at the anode.
[0035] The usefulness and desirability of lithium compounds is tempered by lithium's expense. Lithium and lithium compounds are much more expensive than other alkali or alkaline earth metals and their compounds. Further studies seeking appropriate compounds included using a variety of magnesium compounds. The compositions of some of the mixtures tested are listed in Table 2.
Table 2 Chemical composition of Solid Methanol Fuels using Magnesium Compounds as Additives Fuel I.D. # Mg compounds, Solid Methanol wt% Comment Wt%
1 Mg(OH)2, 64.36 35.64 Solid paste 2 MgO, 56 44 Solid paste 3 Mg(OCH3)2, 100 0 Solid crystal 4 Mg, 42.2 57.6 Solid paste [0036] The tests involved using magnesium compounds either alone, as in the case of magnesium methoxide (Mg(OCH3)2), or as a mixture with solid methanol. The solid methanol comprised a mixture of methanol and Carbopol 981. Figures 3-6 show the results of tests using magnesium or various magnesium compounds with solid methanol in fuel cells. The magnesium compounds include, but are not limited to, magnesium hydroxide (Mg(OH)2), magnesium oxide (MgO), magnesium methoxide (Mg(OCH3)2), and magnesium hydride (MgH2). The figures present the I-V, or current vs. potential, curves measured for various compositions. In the tests a small amount of water was added to create humidity in the anode chamber. The reactions of the solid fuel are initiated with a small amount of humidity, and then can be self generating as the reaction at the anode generates moisture.
The magnesium compounds also adsorb the carbon dioxide (C02) generated at the anode when the methanol reacts to generate an electrical current.
Table 2 Chemical composition of Solid Methanol Fuels using Magnesium Compounds as Additives Fuel I.D. # Mg compounds, Solid Methanol wt% Comment Wt%
1 Mg(OH)2, 64.36 35.64 Solid paste 2 MgO, 56 44 Solid paste 3 Mg(OCH3)2, 100 0 Solid crystal 4 Mg, 42.2 57.6 Solid paste [0036] The tests involved using magnesium compounds either alone, as in the case of magnesium methoxide (Mg(OCH3)2), or as a mixture with solid methanol. The solid methanol comprised a mixture of methanol and Carbopol 981. Figures 3-6 show the results of tests using magnesium or various magnesium compounds with solid methanol in fuel cells. The magnesium compounds include, but are not limited to, magnesium hydroxide (Mg(OH)2), magnesium oxide (MgO), magnesium methoxide (Mg(OCH3)2), and magnesium hydride (MgH2). The figures present the I-V, or current vs. potential, curves measured for various compositions. In the tests a small amount of water was added to create humidity in the anode chamber. The reactions of the solid fuel are initiated with a small amount of humidity, and then can be self generating as the reaction at the anode generates moisture.
The magnesium compounds also adsorb the carbon dioxide (C02) generated at the anode when the methanol reacts to generate an electrical current.
[0037] - An alternate solid fuel studied was acetaldehyde solid fuel. The fuel comprised a mixture of 50 gm of acetaldehyde and 0.5 gm of Carbopol 981. The fuel was allowed to gel and the solid fuel was mixed with 3.2 gm of magnesium oxide. The I-V curve of solid acetaldehyde with MgO was measured and compared with the results for solid methanol with MgO. The results are shown in Figure 7, showing an improvement over the solid methanol.
[0038] In addition to the solid oxygenate fuels, it was found that perfonnance of the fuels can be enhanced with the addition of an oxidant. Especially, an oxidant that generates hydrogen in the process of activating the fuel. Direct methanol fuel cells were studied with oxidants in pulse mode. After a pulse of oxidant, in this case hydrogen peroxide (H202), was added, the fuel cell exhibited a dilution effect, but then there was an increase in the power density, as can be seen in Figure 8. There was an ultimate improvement of 14%
in the power density. Hydrogen peroxide solutions from 1 to 3 weight percent were added to 3 weight percent methanol solutions, and the I-V curves were measured. An improvement was found in the I-V curves by the addition of an oxidant to the methanol as shown in Figure 9. For hydrogen peroxide, the addition of a 2 weight percent solution showed the greatest improvement.
in the power density. Hydrogen peroxide solutions from 1 to 3 weight percent were added to 3 weight percent methanol solutions, and the I-V curves were measured. An improvement was found in the I-V curves by the addition of an oxidant to the methanol as shown in Figure 9. For hydrogen peroxide, the addition of a 2 weight percent solution showed the greatest improvement.
[0039] Although hydrogen peroxide is a liquid, solid oxidants having comparable behavior are available. Alternate oxidants include, but are not limited to, sodium percarbonate, carbamide hydrogen peroxide, organic peroxides, such as tert-butyl hydroperoxide (TBHP), tert-pentyl hydroperoxide, etc., and alkaline earth metal peroxides such as magnesium peroxide and calcium peroxide.
[0040] The addition of strong oxidizing agents has been further studied to determine the influence on power generation for direct methanol fuel cells. Tests were run in pulse mode with an injection of sulfuric acid (H2S04) to solid methanol. The sulfuric acid addition generated additional hydrogen from the magnesium metal and improved the DMFC
performance. The results shown in Figures 10-12, show an improvement in the power density, and increases in the pressure in the anode compartment of the fuel cell.
Additional acids which can be used include, but are not limited to, hydrochloric acid (HCl), and nitric acid (HN 3).
performance. The results shown in Figures 10-12, show an improvement in the power density, and increases in the pressure in the anode compartment of the fuel cell.
Additional acids which can be used include, but are not limited to, hydrochloric acid (HCl), and nitric acid (HN 3).
[0041] The addition of oxidizing agents improves performance and such oxidizing agents can be added in a solid form, where the oxidizing agent reacts with the solid fuel when in the presence of moisture. The control of the addition of water to the fuel can be used to control the generation of gaseous fuel for the fuel cell and allow for intermittent power generation. As an alternative, a strong liquid oxidizing agent can be held in a separate and sealed compartment for controlled addition to a solid fuel when the fuel is placed in fluid communication with the anode compartment of the fuel cell.
[0042] Another aspect with the addition of compounds such as peroxides, is the heat release when the peroxide reacts, or decomposes. The heat release facilitates the vaporization of methanol, or other organic compound that reacts at the anode of the fuel cell in a gaseous phase. The decomposition of the peroxide can be facilitated by the addition of a small amount of catalyst. The catalyst for the decomposition of the oxidizer is a compound comprising one or more metals selected from calcium (Ca), scandium (Sc), titanium (Ti), vanadium (V), chromium (Cr), manganese (Mn), iron (Fe), cobalt (Co), nickel (Ni), copper (Cu), zinc (Zn), strontium (Sr), yttrium (Y), zirconium (Zr), niobium (Nb), molybdenum (Mo), technetium (Tc), ruthenium (Ru), rhodium (Rh), palladium (Pd), silver (Ag), cadmium (Cd), barium (Ba), lanthanum (La), hafnium (Hf), tantalum (Ta), tungsten (W), rhenium (Re), osmium (Os), iridium (Ir), platinum (Pt), gold (Au), and mercury (Hg). The catalyst can include oxides of the metal, sulfides and other sulfur compounds of the metal and sols comprising the metal.
Preferred catalysts comprise one or more metals from vanadium, iron, cobalt, ruthenium, copper, nickel, manganese, molybdenum, platinum, gold, silver, palladium, rhodium, rhenium, osmium, and iridium, with the more preferred catalyst comprising iron, cobalt, nickel and manganese. A more preferred compound is manganese oxide (MnOz).
[0043] While the invention has been described with what are presently considered the preferred embodiments, it is to be understood that the invention is not limited to the disclosed embodiments, but it is intended to cover various modifications and equivalent arrangements included within the scope of the appended claims.
Preferred catalysts comprise one or more metals from vanadium, iron, cobalt, ruthenium, copper, nickel, manganese, molybdenum, platinum, gold, silver, palladium, rhodium, rhenium, osmium, and iridium, with the more preferred catalyst comprising iron, cobalt, nickel and manganese. A more preferred compound is manganese oxide (MnOz).
[0043] While the invention has been described with what are presently considered the preferred embodiments, it is to be understood that the invention is not limited to the disclosed embodiments, but it is intended to cover various modifications and equivalent arrangements included within the scope of the appended claims.
Claims (10)
1. A solid fuel for generating a gaseous fuel for use in a fuel cell, comprising:
an oxygenate compound selected from the group consisting of metal oxygenates, gel led oxygenates, frozen oxygenates, and mixtures thereof; and a solid oxidant selected from the group consisting of sodium percarbonate, carbamide hydrogen peroxide, organic peroxides, and mixtures thereof.
an oxygenate compound selected from the group consisting of metal oxygenates, gel led oxygenates, frozen oxygenates, and mixtures thereof; and a solid oxidant selected from the group consisting of sodium percarbonate, carbamide hydrogen peroxide, organic peroxides, and mixtures thereof.
2. The solid fuel of claim 1 wherein the oxygenate is selected from the group consisting of alcohols, aldehydes, organic acids, ethers, diols, triols, ketones, diketones, esters, carbonates, oxalates, sugars, metal alkoxides, metal aldehydes, and mixtures thereof.
3. (Cancelled)
4. The solid fuel of any of the claims 1 or 2 wherein the gelled oxygenate comprises:
an oxygenate; and a polymeric mixture selected from the group consisting of acrylic acid based polymers, acrylic amide based polymers, copolymers of polyols, copolymers of oligomers containing OH
groups with formaldehyde, ethylene/acrylic acid copolymers with amine emulsifiers, carbonyl vinyl polymers, polyacrylic acid polymers, olefin-maleic anhydride copolymers, and mixtures thereof.
an oxygenate; and a polymeric mixture selected from the group consisting of acrylic acid based polymers, acrylic amide based polymers, copolymers of polyols, copolymers of oligomers containing OH
groups with formaldehyde, ethylene/acrylic acid copolymers with amine emulsifiers, carbonyl vinyl polymers, polyacrylic acid polymers, olefin-maleic anhydride copolymers, and mixtures thereof.
5. The solid fuel of claim 4 wherein the gelled oxygenate comprises:
an oxygenate selected from the group consisting of methanol, acetaldehyde, and mixtures thereof, wherein the oxygenate is in an amount of at least 30 weight percent; and an acrylic polymer in an amount of at least 3 weight percent.
an oxygenate selected from the group consisting of methanol, acetaldehyde, and mixtures thereof, wherein the oxygenate is in an amount of at least 30 weight percent; and an acrylic polymer in an amount of at least 3 weight percent.
6. The solid fuel of claims 1 or 2 or 4, or 5 wherein the gelled oxygenate further comprises a metal or metal compound, where the metal is selected from the group consisting of alkali metals, alkaline earth metals, and mixtures thereof.
7. The solid fuel of claim 6 wherein the metal or metal compound is selected from the group consisting of magnesium hydroxide (Mg(OH)2), magnesium oxide (MgO), magnesium methoxide (Mg(OCH3)2), magnesium (Mg), magnesium hydride (MgH2), and mixtures thereof.
8. The solid fuel of any of claims 1 or 2 or 4 or 5, or 6 further comprising a solid catalyst selected from the group consisting of transition metals, oxides of transition metals, and mixtures thereof.
9. The solid fuel of claim 1 wherein the metal oxygenate comprises a metal selected from the group consisting of lithium (Li), sodium (Na), potassium (K), beryllium (Be), magnesium (Mg), calcium (Ca), rubidium (Rb), cesium (Cs), strontium (Sr), barium (Ba), aluminum (Al), and mixtures thereof.
10. The solid fuel of claim 9 wherein the metal is selected from the group consisting of lithium, sodium, potassium, magnesium, and mixtures thereof.
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PCT/US2004/037099 WO2006052243A1 (en) | 2004-11-05 | 2004-11-05 | Solid fuels for fuel cells |
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JP (1) | JP2008519418A (en) |
CN (1) | CN100492739C (en) |
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BR (1) | BRPI0419137A (en) |
CA (1) | CA2586465A1 (en) |
IL (1) | IL182759A0 (en) |
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JP5163844B2 (en) * | 2006-10-11 | 2013-03-13 | 栗田工業株式会社 | Fuel supply method, fuel cell system, and portable electronic device |
JP5206758B2 (en) * | 2010-07-15 | 2013-06-12 | トヨタ自動車株式会社 | Negative electrode material, metal secondary battery, and negative electrode material manufacturing method |
EP2822607B1 (en) | 2012-03-09 | 2023-06-07 | B.C.B. International Limited | Alcohol-containing compositions useful as solid fuels and processes for their manufacture |
CN105428673A (en) * | 2015-11-26 | 2016-03-23 | 中国科学院上海高等研究院 | Fuel supply system of passive direct methanol fuel cell |
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US7128106B2 (en) * | 2003-04-15 | 2006-10-31 | The Gillette Company | Apparatus for refueling a direct oxidation fuel cell |
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- 2004-11-05 AU AU2004324847A patent/AU2004324847A1/en not_active Abandoned
- 2004-11-05 EP EP04800852A patent/EP1807898A1/en not_active Withdrawn
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- 2004-11-05 CA CA002586465A patent/CA2586465A1/en not_active Abandoned
- 2004-11-05 CN CNB2004800443682A patent/CN100492739C/en not_active Expired - Fee Related
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IL182759A0 (en) | 2007-07-24 |
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EP1807898A1 (en) | 2007-07-18 |
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CN100492739C (en) | 2009-05-27 |
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