JP6289797B2 - 選択的アンモニア酸化のための二元金属触媒 - Google Patents
選択的アンモニア酸化のための二元金属触媒 Download PDFInfo
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- JP6289797B2 JP6289797B2 JP2011534869A JP2011534869A JP6289797B2 JP 6289797 B2 JP6289797 B2 JP 6289797B2 JP 2011534869 A JP2011534869 A JP 2011534869A JP 2011534869 A JP2011534869 A JP 2011534869A JP 6289797 B2 JP6289797 B2 JP 6289797B2
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- catalyst
- copper
- platinum
- ammonia
- molecular sieve
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- 239000003054 catalyst Substances 0.000 title claims description 194
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 title claims description 124
- 229910021529 ammonia Inorganic materials 0.000 title claims description 62
- 238000007254 oxidation reaction Methods 0.000 title claims description 42
- 230000003647 oxidation Effects 0.000 title claims description 41
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 156
- 239000010949 copper Substances 0.000 claims description 87
- 229910052802 copper Inorganic materials 0.000 claims description 72
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical group [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 62
- 239000000758 substrate Substances 0.000 claims description 55
- 229910052697 platinum Inorganic materials 0.000 claims description 50
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 42
- 239000002808 molecular sieve Substances 0.000 claims description 41
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 41
- 239000010457 zeolite Substances 0.000 claims description 39
- 238000000034 method Methods 0.000 claims description 38
- 229910021536 Zeolite Inorganic materials 0.000 claims description 36
- 229910052751 metal Inorganic materials 0.000 claims description 34
- 239000002184 metal Substances 0.000 claims description 34
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 32
- 238000005342 ion exchange Methods 0.000 claims description 31
- 239000002243 precursor Substances 0.000 claims description 28
- 239000007789 gas Substances 0.000 claims description 24
- 230000009467 reduction Effects 0.000 claims description 20
- 239000002245 particle Substances 0.000 claims description 16
- 239000000377 silicon dioxide Substances 0.000 claims description 16
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 14
- 238000011068 loading method Methods 0.000 claims description 13
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 9
- 229910000323 aluminium silicate Inorganic materials 0.000 claims description 6
- 229910052757 nitrogen Inorganic materials 0.000 claims description 6
- 238000004891 communication Methods 0.000 claims description 5
- 230000006378 damage Effects 0.000 claims description 3
- 238000002347 injection Methods 0.000 claims description 3
- 239000007924 injection Substances 0.000 claims description 3
- 238000011144 upstream manufacturing Methods 0.000 claims description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims 1
- 239000010931 gold Substances 0.000 claims 1
- 229910052737 gold Inorganic materials 0.000 claims 1
- 239000011214 refractory ceramic Substances 0.000 claims 1
- 238000006243 chemical reaction Methods 0.000 description 30
- 230000000694 effects Effects 0.000 description 20
- 238000006722 reduction reaction Methods 0.000 description 17
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 17
- 239000002002 slurry Substances 0.000 description 16
- 230000032683 aging Effects 0.000 description 15
- 239000000203 mixture Substances 0.000 description 14
- 239000000463 material Substances 0.000 description 13
- 230000008569 process Effects 0.000 description 13
- 230000007423 decrease Effects 0.000 description 11
- 230000000052 comparative effect Effects 0.000 description 10
- 239000007787 solid Substances 0.000 description 10
- 238000001354 calcination Methods 0.000 description 9
- 150000001875 compounds Chemical class 0.000 description 9
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 8
- 230000003197 catalytic effect Effects 0.000 description 8
- 150000002739 metals Chemical class 0.000 description 8
- 239000000725 suspension Substances 0.000 description 8
- 238000013461 design Methods 0.000 description 7
- 239000000243 solution Substances 0.000 description 7
- JPVYNHNXODAKFH-UHFFFAOYSA-N Cu2+ Chemical compound [Cu+2] JPVYNHNXODAKFH-UHFFFAOYSA-N 0.000 description 6
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 6
- 239000008367 deionised water Substances 0.000 description 6
- 229910021641 deionized water Inorganic materials 0.000 description 6
- 230000001590 oxidative effect Effects 0.000 description 6
- 238000002360 preparation method Methods 0.000 description 6
- 239000000047 product Substances 0.000 description 6
- 241000894007 species Species 0.000 description 6
- -1 tetrachloroplatinum (II) salt Chemical class 0.000 description 6
- 229910045601 alloy Inorganic materials 0.000 description 5
- 239000000956 alloy Substances 0.000 description 5
- NOWPEMKUZKNSGG-UHFFFAOYSA-N azane;platinum(2+) Chemical compound N.N.N.N.[Pt+2] NOWPEMKUZKNSGG-UHFFFAOYSA-N 0.000 description 5
- 229910001431 copper ion Inorganic materials 0.000 description 5
- 238000005470 impregnation Methods 0.000 description 5
- 238000004519 manufacturing process Methods 0.000 description 5
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 5
- 239000011148 porous material Substances 0.000 description 5
- 239000000843 powder Substances 0.000 description 5
- 150000003839 salts Chemical class 0.000 description 5
- 239000002904 solvent Substances 0.000 description 5
- 238000003917 TEM image Methods 0.000 description 4
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 4
- 238000013459 approach Methods 0.000 description 4
- 238000000576 coating method Methods 0.000 description 4
- OPQARKPSCNTWTJ-UHFFFAOYSA-L copper(ii) acetate Chemical compound [Cu+2].CC([O-])=O.CC([O-])=O OPQARKPSCNTWTJ-UHFFFAOYSA-L 0.000 description 4
- 229910052878 cordierite Inorganic materials 0.000 description 4
- 239000013078 crystal Substances 0.000 description 4
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 description 4
- 229910001873 dinitrogen Inorganic materials 0.000 description 4
- 229910052742 iron Inorganic materials 0.000 description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 3
- GQPLMRYTRLFLPF-UHFFFAOYSA-N Nitrous Oxide Chemical compound [O-][N+]#N GQPLMRYTRLFLPF-UHFFFAOYSA-N 0.000 description 3
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 3
- 238000004458 analytical method Methods 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- 239000006227 byproduct Substances 0.000 description 3
- 239000004202 carbamide Substances 0.000 description 3
- 229910002091 carbon monoxide Inorganic materials 0.000 description 3
- 238000010531 catalytic reduction reaction Methods 0.000 description 3
- 239000000919 ceramic Substances 0.000 description 3
- 239000011248 coating agent Substances 0.000 description 3
- 239000006185 dispersion Substances 0.000 description 3
- 238000001914 filtration Methods 0.000 description 3
- 239000012530 fluid Substances 0.000 description 3
- 229930195733 hydrocarbon Natural products 0.000 description 3
- 150000002430 hydrocarbons Chemical class 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 230000003993 interaction Effects 0.000 description 3
- 150000002500 ions Chemical group 0.000 description 3
- 229910052759 nickel Inorganic materials 0.000 description 3
- 229910052845 zircon Inorganic materials 0.000 description 3
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 description 3
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 2
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical compound [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 description 2
- 239000005751 Copper oxide Substances 0.000 description 2
- 241000264877 Hippospongia communis Species 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 2
- 229910052782 aluminium Inorganic materials 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 125000002091 cationic group Chemical group 0.000 description 2
- 239000003638 chemical reducing agent Substances 0.000 description 2
- 229910052804 chromium Inorganic materials 0.000 description 2
- 239000011651 chromium Substances 0.000 description 2
- 239000006255 coating slurry Substances 0.000 description 2
- 229910000431 copper oxide Inorganic materials 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 238000011156 evaluation Methods 0.000 description 2
- 229910001092 metal group alloy Inorganic materials 0.000 description 2
- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- 230000003278 mimic effect Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 239000012452 mother liquor Substances 0.000 description 2
- 239000013618 particulate matter Substances 0.000 description 2
- 230000000737 periodic effect Effects 0.000 description 2
- 150000003057 platinum Chemical class 0.000 description 2
- NFOHLBHARAZXFQ-UHFFFAOYSA-L platinum(2+);dihydroxide Chemical compound O[Pt]O NFOHLBHARAZXFQ-UHFFFAOYSA-L 0.000 description 2
- KIDPOJWGQRZHFM-UHFFFAOYSA-N platinum;hydrate Chemical compound O.[Pt] KIDPOJWGQRZHFM-UHFFFAOYSA-N 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 239000004071 soot Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 239000010936 titanium Substances 0.000 description 2
- 239000003039 volatile agent Substances 0.000 description 2
- VEJOYRPGKZZTJW-FDGPNNRMSA-N (z)-4-hydroxypent-3-en-2-one;platinum Chemical compound [Pt].C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O VEJOYRPGKZZTJW-FDGPNNRMSA-N 0.000 description 1
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 description 1
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 1
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 1
- 239000007848 Bronsted acid Substances 0.000 description 1
- JJLJMEJHUUYSSY-UHFFFAOYSA-L Copper hydroxide Chemical compound [OH-].[OH-].[Cu+2] JJLJMEJHUUYSSY-UHFFFAOYSA-L 0.000 description 1
- 239000005750 Copper hydroxide Substances 0.000 description 1
- 206010015946 Eye irritation Diseases 0.000 description 1
- 229910001200 Ferrotitanium Inorganic materials 0.000 description 1
- 239000002841 Lewis acid Substances 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 1
- 230000010718 Oxidation Activity Effects 0.000 description 1
- 229910052581 Si3N4 Inorganic materials 0.000 description 1
- 206010040880 Skin irritation Diseases 0.000 description 1
- 206010043521 Throat irritation Diseases 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 230000002730 additional effect Effects 0.000 description 1
- 238000003915 air pollution Methods 0.000 description 1
- HEHRHMRHPUNLIR-UHFFFAOYSA-N aluminum;hydroxy-[hydroxy(oxo)silyl]oxy-oxosilane;lithium Chemical compound [Li].[Al].O[Si](=O)O[Si](O)=O.O[Si](=O)O[Si](O)=O HEHRHMRHPUNLIR-UHFFFAOYSA-N 0.000 description 1
- 239000000908 ammonium hydroxide Substances 0.000 description 1
- 125000000129 anionic group Chemical group 0.000 description 1
- 239000010953 base metal Substances 0.000 description 1
- 230000001588 bifunctional effect Effects 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 238000005341 cation exchange Methods 0.000 description 1
- 150000001768 cations Chemical class 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 230000002860 competitive effect Effects 0.000 description 1
- 230000000536 complexating effect Effects 0.000 description 1
- 238000009833 condensation Methods 0.000 description 1
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- 238000010276 construction Methods 0.000 description 1
- 150000001879 copper Chemical class 0.000 description 1
- 229910001956 copper hydroxide Inorganic materials 0.000 description 1
- 229910000365 copper sulfate Inorganic materials 0.000 description 1
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Chemical compound [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 description 1
- ARUVKPQLZAKDPS-UHFFFAOYSA-L copper(II) sulfate Chemical compound [Cu+2].[O-][S+2]([O-])([O-])[O-] ARUVKPQLZAKDPS-UHFFFAOYSA-L 0.000 description 1
- ZKXWKVVCCTZOLD-UHFFFAOYSA-N copper;4-hydroxypent-3-en-2-one Chemical compound [Cu].CC(O)=CC(C)=O.CC(O)=CC(C)=O ZKXWKVVCCTZOLD-UHFFFAOYSA-N 0.000 description 1
- NWFNSTOSIVLCJA-UHFFFAOYSA-L copper;diacetate;hydrate Chemical compound O.[Cu+2].CC([O-])=O.CC([O-])=O NWFNSTOSIVLCJA-UHFFFAOYSA-L 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000008878 coupling Effects 0.000 description 1
- 238000010168 coupling process Methods 0.000 description 1
- 238000005859 coupling reaction Methods 0.000 description 1
- 238000002425 crystallisation Methods 0.000 description 1
- 230000008025 crystallization Effects 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 238000003795 desorption Methods 0.000 description 1
- KZHJGOXRZJKJNY-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Si]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O KZHJGOXRZJKJNY-UHFFFAOYSA-N 0.000 description 1
- 238000000635 electron micrograph Methods 0.000 description 1
- 230000008030 elimination Effects 0.000 description 1
- 238000003379 elimination reaction Methods 0.000 description 1
- 239000012065 filter cake Substances 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 239000005431 greenhouse gas Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000008241 heterogeneous mixture Substances 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
- 239000007788 liquid Substances 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- 229910001947 lithium oxide Inorganic materials 0.000 description 1
- HCWCAKKEBCNQJP-UHFFFAOYSA-N magnesium orthosilicate Chemical compound [Mg+2].[Mg+2].[O-][Si]([O-])([O-])[O-] HCWCAKKEBCNQJP-UHFFFAOYSA-N 0.000 description 1
- 239000000395 magnesium oxide Substances 0.000 description 1
- 239000000391 magnesium silicate Substances 0.000 description 1
- 229910052919 magnesium silicate Inorganic materials 0.000 description 1
- 235000019792 magnesium silicate Nutrition 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
- 230000007246 mechanism Effects 0.000 description 1
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- 230000005012 migration Effects 0.000 description 1
- 238000003801 milling Methods 0.000 description 1
- 150000007522 mineralic acids Chemical class 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 229910052863 mullite Inorganic materials 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 239000001272 nitrous oxide Substances 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 150000007524 organic acids Chemical class 0.000 description 1
- WXIWSQBJNUSTTO-UHFFFAOYSA-N pentane-2,4-dione;platinum Chemical compound [Pt].CC(=O)CC(C)=O.CC(=O)CC(C)=O WXIWSQBJNUSTTO-UHFFFAOYSA-N 0.000 description 1
- 229910052670 petalite Inorganic materials 0.000 description 1
- CLSUSRZJUQMOHH-UHFFFAOYSA-L platinum dichloride Chemical compound Cl[Pt]Cl CLSUSRZJUQMOHH-UHFFFAOYSA-L 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 229910052611 pyroxene Inorganic materials 0.000 description 1
- 239000011819 refractory material Substances 0.000 description 1
- 239000003870 refractory metal Substances 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 230000036556 skin irritation Effects 0.000 description 1
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- 230000007928 solubilization Effects 0.000 description 1
- 238000005063 solubilization Methods 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
- 239000003381 stabilizer Substances 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 230000000153 supplemental effect Effects 0.000 description 1
- 239000004094 surface-active agent Substances 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
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- 229910052719 titanium Inorganic materials 0.000 description 1
- 238000012546 transfer Methods 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
- 239000002699 waste material Substances 0.000 description 1
- 239000010456 wollastonite Substances 0.000 description 1
- 229910052882 wollastonite Inorganic materials 0.000 description 1
Images
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8621—Removing nitrogen compounds
- B01D53/8634—Ammonia
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
- B01D53/9404—Removing only nitrogen compounds
- B01D53/9436—Ammonia
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/064—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof containing iron group metals, noble metals or copper
- B01J29/068—Noble metals
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/064—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof containing iron group metals, noble metals or copper
- B01J29/072—Iron group metals or copper
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/08—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y
- B01J29/10—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y containing iron group metals, noble metals or copper
- B01J29/14—Iron group metals or copper
- B01J29/146—Y-type faujasite
-
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Description
4NH3+5O2→4NO+6H2O 式1
4NOx+4NH3+(3−2x)O2→4N2+6H2O 式2
2つの他の第2のプロセスは、アンモニア酸化触媒の選択性を決定することにおいて重要である。式3に従って、亜酸化窒素(N2O)がNOから産生でき、式4に従って、NO2が産生できる。
2NOx+→N2O+(2x-1)/2O2 式3
NO+1/2O2→NO2 式4
式1〜式4の全ては、支持されているPt触媒によって通常触媒され、異なる温度でのこれらのプロセスの相対的比率は酸化生成物の分布を定める。式2はSCRプロセスと同等であり、銅を含有するモレキュラーシーブを含む多数の既知のSCR触媒のいずれかによって触媒されるであろう。触媒する式2の成分の包含は、概して触媒の正味N2選択性を上昇する効果を有するであろう。本発明の幾つかの実施形態において、式2を触媒するための追加の成分は触媒ウォッシュコート中に含まれるであろう。特定の実施形態において、式2を触媒するための成分は銅交換モレキュラーシーブであるであろう。さらにより具体的な実施形態において、PGMは銅交換モレキュラーシーブ上または銅交換モレキュラーシーブ中に直接支持されるであろう。
1つ以上の実施形態に従うと、アンモニア酸化触媒のための基材は、典型的に自動車用触媒の調製のために使用されるそれらの材料のいずれであってもよく、金属またはセラミックハニカム構造を典型的には含むであろう。通路を流体流動に対して開くように、基材の入口から出口面へと延在している複数の微細で平行なガス流通路を有するモノリスフロースルー基材等の、いずれの好適な基材も用いられ得る。それらの流体入口からそれらの流体出口まで本質的に直線路である通路は、壁によって画定され、通路を通って流れるガスが触媒材料に接触するように、その壁上に触媒材料はウォッシュコートとしてコーティングされる。モノリス基材の流路は、台形、長方形、正方形、正弦曲線、六角形、長円形、円形等の任意の好適な断面形状でもあり得る薄壁チャネルである。かかる構造は、断面積の1平方インチにつき約60〜約1200以上のガス入口開口部(すなわち、「セル」)(cpsi)を含有し得る。代表的な市販のフロースルー基材はCorning400/6菫青石材料であり、それは菫青石から構築され、400cpsiであり、かつ6ミルの壁の厚さを有する。しかしながら、本発明が特定の基材タイプ、材料、または幾何学的形状に限定されないことが理解されるであろう。
本発明がいずれの特定の理論にも束縛されるものではないが、触媒の1つ以上の実施形態は、以下の仮説に基づいて設計される。(1)NOは、式1に従うNH3酸化の初期の生成物であり、正味NH3転換はこのプロセスに対する比率によって決定付けられる、(2)式2〜式4に従って、NOは、全ての他の窒素生成種へと導く一般的な中間体であり、N2選択性は、NO中間体を含むこれらの第2の反応イオンの相対的比率によって決定付けられる、(3)それ自体が良きSCR触媒であるPGM支持体の利用は追加の化学反応チャネルを開き、これは式2の正味比率を上昇させ、それによってN2の形成を助ける。これらの仮説はともに、選択的アンモニア酸化触媒の設計のための一般的パラダイムを示唆し、そこではPGMが、SCR成分上に支持されるか、あるいはSCR成分と直接関連付けられる。このアプローチは、ニ機能性NH3酸化触媒の設計に対する代替的なアプローチとは異なる、そこではPGMは、SCR成分から化学的および物理的に独立している支持体上に設置される。前者のアプローチは、後者のものを越える幾つかの利点を有する。これは、単一のウォッシュコート層のみが必要とされるため、触媒製造を単純化する。壁流フィルター等の2つの触媒層が実行可能でない状況において、直ちに受け入れられる。最後に、それは、近い物理的近接(同一支持体上)における全ての触媒機能を設置し、所望のN2生成物への選択性を改善する。
1つ以上の実施形態に従うと、触媒は、基材上に堆積された、すなわち、基材上にコーティングされ、かつ接着されたウォッシュコート層として塗布される。基材に触媒層を塗布するため、白金成分および/または金属ゼオライト成分を含む触媒の微細に分割された粒子は、スラリーを形成するため適切な溶媒(例えば、水)中に懸濁される。他のプロモーターおよび/または安定剤および/または界面活性剤は、水または水混和性溶媒中で、混合物または溶液としてスラリーに添加され得る。1つ以上の実施形態において、スラリーは、結果として、実質的に全ての固体が、約10ミクロン未満の粒子サイズ、すなわち約0.1〜8ミクロンの平均直径を有するように、粉末状にされる。粉砕は、ボールミル、連続的アイガーミル、または他の同様の装置において達成され得る。1つ以上の実施形態において、懸濁液またはスラリーは、約2〜約7未満のpHを有する。スラリーのpHは、適切な量の無機または有機酸のスラリーへの添加によって、必要ならば調整され得る。銅を配位させ、かつ動かし得るいかなる種もスラリーに添加されていないことに注意するべきである。スラリーの固体含有量は、例えば、約20〜60重量%、より具体的には約35〜45重量%であり得る。所望の装填量の触媒層を基材上に堆積するように、基材は、次いでスラリー中に浸漬され得、あるいはスラリーが基材上にコーティングされ得る。その後、コーティングされた基材は約100℃で乾燥され、例えば、300〜650℃で約1〜約3時間、加熱によって焼成される。乾燥および焼成は、典型的には空気中で行われる。コーティング、乾燥、および焼成プロセスは、支持体上で触媒の最終所望の装填量を達成するため、必要であれば繰り返され得る。幾つかの場合において、液体および他の揮発性成分の完全除去は、触媒が使用に設置され、操作の間に遭遇する高温に供されるまで、生じ得ない。
本発明の1つ以上の実施形態に従うと、希薄燃焼車両またはディーゼル車両の排気ガス流中の産生された排出物を処理するための方法が提供される。1つ以上の実施形態のNOx低減触媒は、選択的触媒還元(SCR)触媒、またはNOx低減触媒からの可能性があるアンモニアの排出またはスリップをもたらすNOxの破壊のための他の触媒を含む。
ゼオライト触媒上のPt+Cuの一般的調製が、Cu2+の連続的イオン交換、続いてカチオン白金錯体によって達成された。一実施例において、銅交換されたY−ゼオライトを、第1に、75gの(375mmol)酢酸銅水和物を1250mLの脱イオン水中に溶解することによって調製し、全ての酢酸銅が溶解したことを確認した。青色の溶液を得るため、500g(揮発性物質を含まない固体基準)のZeolyst CBV500Yタイプゼオライトをゆっくりと添加し、懸濁液中に約30重量%の固体含有量を得た。pHを4.5(±0.1)に調製し、懸濁液を室温で24時間撹拌した。pHを4.5(±0.1)に再調製し、試料をさらに1時間撹拌した。固体を濾過によって収集し、再懸濁し、10分間撹拌し、次いで濾過によって再収集した。得られたフィルターケークを脱イオン水で3回洗浄した。湿った粉末を130℃で一晩乾燥し、次いで640℃で1時間焼成した。焼成した固体の組成物分析は3.0%(揮発性物質を含まない、銅金属基準)の銅含有量を与えた。
Claims (9)
- アンモニアを窒素およびNOxに酸化するための触媒であって、前記触媒は、6未満のシリカ/アルミナ比(SAR)を有するアルミノケイ酸塩モレキュラーシーブを含み、且つ当該モレキュラーシーブは銅および白金の両方を含み、及び
前記白金は、ゼロ原子価または金属白金を所定量で含み、
前記ゼロ原子価または金属白金は、よく面が切り出された粒子の状態であり、該粒子は10〜50nmの粒径を有し、及び
前記白金及び前記銅の活性部位が物理的に分離されたまま残存することを特徴とする触媒。 - 前記アルミノケイ酸塩モレキュラーシーブは、FAU、MFI、MOR、BEA、HEU、およびOFFから選択される結晶骨格型を有するゼオライトを含む、請求項1に記載の触媒。
- ウォッシュコート当たりの重量基準で、1重量%以下のPtおよび5重量%以下の銅を有する、請求項1に記載の触媒。
- 前記触媒は、耐火性セラミック担体上にコーティングされる、請求項1に記載の触媒。
- 前記基材上の前記モレキュラーシーブの総装填量は、総触媒量に基づいて0.3g/in3〜3.0g/in3[(0.3/25.43)g/mm3〜(3.0/25.43)g/mm3]の範囲である、請求項4に記載の触媒。
- ディーゼルまたは希薄燃焼車両の排気ガス流中に生成した排出物を処理するための方法であって、前記方法は、
車両のエンジン排気流を少なくともNOx低減触媒を通過させる工程、
前記NOx低減触媒から出たアンモニア含有前記排気流を、酸化触媒を通過させる工程を含み、
前記酸化触媒は、15未満のシリカ/アルミナ比(SAR)を有するモレキュラーシーブを含み、及び当該モレキュラーシーブは焼成されたイオン交換銅およびイオン交換白金の両方を含んでいることを特徴とする方法。 - 前記NOx低減触媒は、SCR触媒、希薄NOx捕捉触媒、または前記NOx低減触媒からのアンモニアスリップをもたらすNOxの破壊のための他の触媒のうちの1つ以上から選択される、請求項6に記載の方法。
- 前記モレキュラーシーブはゼオライトを含む、請求項7に記載の方法。
- 排気ガス流を処理するためのシステムであって、
前記排気ガス流と連通するSCR触媒と、
前記排気ガス流と連通し、前記SCR触媒から上流に位置するアンモニアまたはアンモニア前駆体注入ポートと、
前記排気ガス流と連通し、前記SCR触媒から下流に位置する、請求項1に記載の触媒と、を含む、システム。
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US8596063B2 (en) * | 2009-06-18 | 2013-12-03 | GM Global Technology Operations LLC | Exhaust treatment system for an internal combustion engine |
RU2572610C2 (ru) * | 2010-11-02 | 2016-01-20 | Хальдор Топсеэ А/С | Способ получения катализируемого сажевого фильтра и катализируемый сажевый фильтр |
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BRPI0921502B1 (pt) | 2018-07-03 |
WO2010062733A3 (en) | 2010-07-29 |
KR102126248B1 (ko) | 2020-06-24 |
EP2364211A4 (en) | 2012-08-08 |
EP2364211A2 (en) | 2011-09-14 |
US20100111791A1 (en) | 2010-05-06 |
BRPI0921502A2 (pt) | 2016-09-27 |
EP3854479A1 (en) | 2021-07-28 |
WO2010062733A2 (en) | 2010-06-03 |
JP2012507400A (ja) | 2012-03-29 |
KR20110086720A (ko) | 2011-07-29 |
CN107051574B (zh) | 2021-02-19 |
US20200222853A1 (en) | 2020-07-16 |
CN102271810A (zh) | 2011-12-07 |
KR20170095405A (ko) | 2017-08-22 |
CN107051574A (zh) | 2017-08-18 |
US10632423B2 (en) | 2020-04-28 |
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