JP4443226B2 - FCC法に使用するためのNOx低減用組成物 - Google Patents
FCC法に使用するためのNOx低減用組成物 Download PDFInfo
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- JP4443226B2 JP4443226B2 JP2003547547A JP2003547547A JP4443226B2 JP 4443226 B2 JP4443226 B2 JP 4443226B2 JP 2003547547 A JP2003547547 A JP 2003547547A JP 2003547547 A JP2003547547 A JP 2003547547A JP 4443226 B2 JP4443226 B2 JP 4443226B2
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- 239000000203 mixture Substances 0.000 title claims description 79
- 238000000034 method Methods 0.000 title claims description 42
- 239000003054 catalyst Substances 0.000 claims description 71
- 239000002245 particle Substances 0.000 claims description 46
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 45
- 238000004231 fluid catalytic cracking Methods 0.000 claims description 45
- 230000002378 acidificating effect Effects 0.000 claims description 27
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 26
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 claims description 26
- 238000005336 cracking Methods 0.000 claims description 22
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 20
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 18
- 229910052723 transition metal Inorganic materials 0.000 claims description 14
- 150000003624 transition metals Chemical class 0.000 claims description 14
- 229930195733 hydrocarbon Natural products 0.000 claims description 13
- 150000002430 hydrocarbons Chemical class 0.000 claims description 13
- 239000000377 silicon dioxide Substances 0.000 claims description 10
- 239000005995 Aluminium silicate Substances 0.000 claims description 9
- 239000004215 Carbon black (E152) Substances 0.000 claims description 9
- 235000012211 aluminium silicate Nutrition 0.000 claims description 9
- 238000001354 calcination Methods 0.000 claims description 9
- NLYAJNPCOHFWQQ-UHFFFAOYSA-N kaolin Chemical compound O.O.O=[Al]O[Si](=O)O[Si](=O)O[Al]=O NLYAJNPCOHFWQQ-UHFFFAOYSA-N 0.000 claims description 9
- 229910052757 nitrogen Inorganic materials 0.000 claims description 9
- 239000003518 caustics Substances 0.000 claims description 8
- 229910052747 lanthanoid Inorganic materials 0.000 claims description 8
- 150000002602 lanthanoids Chemical class 0.000 claims description 8
- 239000004005 microsphere Substances 0.000 claims description 8
- 229910052684 Cerium Inorganic materials 0.000 claims description 7
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims description 7
- 230000000737 periodic effect Effects 0.000 claims description 7
- 230000008929 regeneration Effects 0.000 claims description 7
- 238000011069 regeneration method Methods 0.000 claims description 7
- 238000004523 catalytic cracking Methods 0.000 claims description 6
- MMKQUGHLEMYQSG-UHFFFAOYSA-N oxygen(2-);praseodymium(3+) Chemical group [O-2].[O-2].[O-2].[Pr+3].[Pr+3] MMKQUGHLEMYQSG-UHFFFAOYSA-N 0.000 claims description 6
- 229910003447 praseodymium oxide Inorganic materials 0.000 claims description 6
- -1 aluminum chlorohydroxide Chemical group 0.000 claims description 4
- 229910052802 copper Inorganic materials 0.000 claims description 4
- 239000010949 copper Substances 0.000 claims description 4
- 238000002386 leaching Methods 0.000 claims description 4
- 229910052709 silver Inorganic materials 0.000 claims description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 2
- 239000012530 fluid Substances 0.000 claims description 2
- 230000003647 oxidation Effects 0.000 claims description 2
- 238000007254 oxidation reaction Methods 0.000 claims description 2
- 238000010438 heat treatment Methods 0.000 claims 2
- 238000000354 decomposition reaction Methods 0.000 claims 1
- 230000001172 regenerating effect Effects 0.000 claims 1
- 239000004332 silver Substances 0.000 claims 1
- 239000000654 additive Substances 0.000 description 23
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 20
- 230000000996 additive effect Effects 0.000 description 17
- 239000000571 coke Substances 0.000 description 12
- 239000000463 material Substances 0.000 description 10
- 229910052777 Praseodymium Inorganic materials 0.000 description 9
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 7
- 229910000311 lanthanide oxide Inorganic materials 0.000 description 7
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 6
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Chemical compound [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 description 6
- 239000011593 sulfur Substances 0.000 description 6
- 229910052717 sulfur Inorganic materials 0.000 description 6
- XTQHKBHJIVJGKJ-UHFFFAOYSA-N sulfur monoxide Chemical compound S=O XTQHKBHJIVJGKJ-UHFFFAOYSA-N 0.000 description 6
- 229910002091 carbon monoxide Inorganic materials 0.000 description 5
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 5
- 229910052751 metal Inorganic materials 0.000 description 5
- 239000002184 metal Substances 0.000 description 5
- 229910017493 Nd 2 O 3 Inorganic materials 0.000 description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 4
- 239000011230 binding agent Substances 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
- TXKMVPPZCYKFAC-UHFFFAOYSA-N disulfur monoxide Inorganic materials O=S=S TXKMVPPZCYKFAC-UHFFFAOYSA-N 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 239000000945 filler Substances 0.000 description 4
- 239000007789 gas Substances 0.000 description 4
- 239000001301 oxygen Substances 0.000 description 4
- 229910052760 oxygen Inorganic materials 0.000 description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 3
- 238000002485 combustion reaction Methods 0.000 description 3
- 239000000446 fuel Substances 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 239000000395 magnesium oxide Substances 0.000 description 3
- 230000014759 maintenance of location Effects 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 229910044991 metal oxide Inorganic materials 0.000 description 3
- 150000004706 metal oxides Chemical class 0.000 description 3
- 229910052596 spinel Inorganic materials 0.000 description 3
- 239000011029 spinel Substances 0.000 description 3
- 238000003860 storage Methods 0.000 description 3
- 239000002912 waste gas Substances 0.000 description 3
- 239000011701 zinc Substances 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- 230000002411 adverse Effects 0.000 description 2
- 229910052783 alkali metal Inorganic materials 0.000 description 2
- 150000001340 alkali metals Chemical class 0.000 description 2
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 2
- 150000001342 alkaline earth metals Chemical class 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 2
- HSJPMRKMPBAUAU-UHFFFAOYSA-N cerium(3+);trinitrate Chemical compound [Ce+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O HSJPMRKMPBAUAU-UHFFFAOYSA-N 0.000 description 2
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 2
- 230000009849 deactivation Effects 0.000 description 2
- 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 2
- 239000003546 flue gas Substances 0.000 description 2
- 239000003502 gasoline Substances 0.000 description 2
- 239000011777 magnesium Substances 0.000 description 2
- YIXJRHPUWRPCBB-UHFFFAOYSA-N magnesium nitrate Chemical compound [Mg+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O YIXJRHPUWRPCBB-UHFFFAOYSA-N 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 229910052863 mullite Inorganic materials 0.000 description 2
- CFYGEIAZMVFFDE-UHFFFAOYSA-N neodymium(3+);trinitrate Chemical compound [Nd+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O CFYGEIAZMVFFDE-UHFFFAOYSA-N 0.000 description 2
- PUDIUYLPXJFUGB-UHFFFAOYSA-N praseodymium atom Chemical compound [Pr] PUDIUYLPXJFUGB-UHFFFAOYSA-N 0.000 description 2
- YWECOPREQNXXBZ-UHFFFAOYSA-N praseodymium(3+);trinitrate Chemical compound [Pr+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O YWECOPREQNXXBZ-UHFFFAOYSA-N 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 239000011734 sodium Substances 0.000 description 2
- VWDWKYIASSYTQR-UHFFFAOYSA-N sodium nitrate Chemical compound [Na+].[O-][N+]([O-])=O VWDWKYIASSYTQR-UHFFFAOYSA-N 0.000 description 2
- 238000001694 spray drying Methods 0.000 description 2
- 229910052815 sulfur oxide Inorganic materials 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 229910052725 zinc Inorganic materials 0.000 description 2
- OHVLMTFVQDZYHP-UHFFFAOYSA-N 1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)-2-[4-[2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidin-5-yl]piperazin-1-yl]ethanone Chemical compound N1N=NC=2CN(CCC=21)C(CN1CCN(CC1)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)=O OHVLMTFVQDZYHP-UHFFFAOYSA-N 0.000 description 1
- 229910021193 La 2 O 3 Inorganic materials 0.000 description 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical group [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000000809 air pollutant Substances 0.000 description 1
- 231100001243 air pollutant Toxicity 0.000 description 1
- 239000011959 amorphous silica alumina Substances 0.000 description 1
- 150000004945 aromatic hydrocarbons Chemical class 0.000 description 1
- 239000002585 base Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 239000004927 clay Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 239000010779 crude oil Substances 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 1
- 238000005470 impregnation Methods 0.000 description 1
- 239000011261 inert gas 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
- 239000007788 liquid Substances 0.000 description 1
- JCCNYMKQOSZNPW-UHFFFAOYSA-N loratadine Chemical compound C1CN(C(=O)OCC)CCC1=C1C2=NC=CC=C2CCC2=CC(Cl)=CC=C21 JCCNYMKQOSZNPW-UHFFFAOYSA-N 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 239000013081 microcrystal Substances 0.000 description 1
- 229910052750 molybdenum Chemical group 0.000 description 1
- 239000011733 molybdenum Chemical group 0.000 description 1
- 229910017464 nitrogen compound Inorganic materials 0.000 description 1
- 150000002830 nitrogen compounds Chemical class 0.000 description 1
- 150000002898 organic sulfur compounds Chemical class 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 239000003209 petroleum derivative Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 238000011946 reduction process Methods 0.000 description 1
- 238000007670 refining Methods 0.000 description 1
- 230000000717 retained effect Effects 0.000 description 1
- 230000035939 shock Effects 0.000 description 1
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 description 1
- 239000010944 silver (metal) Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000004317 sodium nitrate Substances 0.000 description 1
- 235000010344 sodium nitrate Nutrition 0.000 description 1
- 239000011949 solid catalyst Substances 0.000 description 1
- 230000001629 suppression Effects 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical group [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Chemical group 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical group [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G11/00—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
- C10G11/14—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts
- C10G11/18—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts according to the "fluidised-bed" technique
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G11/00—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
- C10G11/02—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils characterised by the catalyst used
- C10G11/04—Oxides
-
- 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
- B01D53/8625—Nitrogen oxides
- B01D53/8628—Processes characterised by a specific catalyst
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/10—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of rare earths
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/83—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with rare earths or actinides
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/90—Regeneration or reactivation
- B01J23/94—Regeneration or reactivation of catalysts comprising metals, oxides or hydroxides of the 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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/19—Catalysts containing parts with different compositions
-
- 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
- B01J38/00—Regeneration or reactivation of catalysts, in general
- B01J38/04—Gas or vapour treating; Treating by using liquids vaporisable upon contacting spent catalyst
- B01J38/12—Treating with free oxygen-containing gas
- B01J38/30—Treating with free oxygen-containing gas in gaseous suspension, e.g. fluidised bed
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
-
- 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
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10S502/00—Catalyst, solid sorbent, or support therefor: product or process of making
- Y10S502/515—Specific contaminant removal
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Materials Engineering (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- General Chemical & Material Sciences (AREA)
- Environmental & Geological Engineering (AREA)
- Biomedical Technology (AREA)
- Analytical Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Catalysts (AREA)
- Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
Description
M2m 2+Al2−pMp 3+TrO7+r・s
をもつ微結晶から実質的に構成された縮約(collapsed)組成物を使用してFCC法におけるガス混合物から酸化硫黄または酸化窒素を除去する方法が記載されている。上記式でM2+は2価の金属、M3+は3価の金属、Tはバナジウム、タングステンまたはモリブデンである。
本発明には、或る種の組成物がFCC法においてNOxガスの放出の低減に極めて有効であるという発見が含まれている。さらに、このような組成物は従来法の組成物に比べ予想外に改善された水熱安定性をもっている。本発明のNOx低減用組成物は(i)酸性酸化物担体、(ii)酸化セリウム、(iii)酸化セリウム以外のランタニド系列の元素の少なくとも1種の酸化物、および(iV)随時含まれる周期律表の第Ib族および第IIb族から選ばれる少なくとも1種の遷移金属の酸化物およびそれらの混合物を含んで成っていることを特徴としている。
(a)酸性酸化物担体粒子を酸化セリウム原料、酸化セリウム以外の少なくとも1種のランタニド酸化物原料、および随時含ませる少なくとも1種の第Ib族/第IIb族元素源で一緒に含浸し、
(b)工程(a)で得た含浸された担体をカ焼する。
2% Pr 6 O 11 /10% CeO 2 /2% CuO/アルミナ
アルミナの担体粒子を、セリウムおよびプラセオジムの硝酸塩の溶液で少し湿らせる程度に(by incipient wetness)一緒に含浸し、乾燥し、1200°Fで2時間カ焼して10重量%のCeO2および2重量%のPr6O11の濃度レベルを得る。微小球体の上で硝酸銅を含浸し、乾燥して1200°Fで2時間カ焼し、2重量%のCuOの濃度レベルを得る。
3% La 2 O 3 /10% CeO 2 /3% Nd 2 O 3 /2% CuO/アルミナ
アルミナの担体粒子を、ランタン、セリウムおよびネオジムの硝酸塩の溶液で少し湿らせる程度に一緒に含浸し、乾燥し、1200°Fで2時間カ焼して10重量%のCeO2および2重量%のNd2O3の濃度レベルを得る。微小球体の上で硝酸銅を含浸し、乾燥して1200°Fで2時間カ焼し、2重量%のCuOの濃度レベルを得る。
2% Pr 6 O 11 /10% CeO 2 /2% CuO/アルミナ
アルミナの担体粒子を、セリウム、プラセオジムおよび銅の硝酸塩の溶液で少し湿らせる程度に一緒に含浸し、乾燥し、1200°Fで2時間カ焼して10%のCeO2/2%のPr6O11/2%のCuOの濃度レベルを得る。
2% Pr 6 O 11 /10% CeO 2 /1.5% Nd 2 O 3 /2% CuO/アルミナ
アルミナの担体粒子を、セリウム、プラセオジムおよびネオジムの硝酸塩の溶液で少し湿らせる程度に一緒に含浸し、乾燥し、1200°Fで2時間カ焼して10%のCeO2/10重量%のPr6O11/1.5%のNd2O3の濃度レベルを得る。この微小球体の上で硝酸銅を含浸し、乾燥して1200°Fで2時間カ焼し、2重量%のCuOの濃度レベルを得る。
3% Na 2 O/10% CeO 2 /2% CuO/アルミナ
アルミナの担体粒子を硝酸ナトリウムで少し湿らせる程度に含浸し、乾燥し、1200°Fで2時間カ焼して3重量%のNa2Oの濃度レベルを得る。Naを含むアルミナ粒子をセリウムおよび銅の硝酸塩の溶液で一緒に含浸し、1200°Fで2時間カ焼し、10重量%のCeO2、2%のCuOの濃度レベルを得る。
5% MgO/10% CeO 2 /2% CuO/アルミナ
アルミナの担体粒子を硝酸マグネシウムで少し湿らせる程度に含浸し、乾燥し、1200°Fで2時間カ焼して5.0%のMgOの濃度レベルを得る。Mgを含むアルミナ粒子をセリウムおよび銅の硝酸塩の溶液で一緒に含浸し、1200°Fで2時間カ焼し、10%のCeO2、2%のCuOの濃度レベルを得る。
10% CeO 2 /アルミナ
アルミナの担体粒子を硝酸セリウムで少し湿らせる程度に含浸し、乾燥し、1200°Fで2時間カ焼して10%のCeO2の濃度レベルを得る。
10% Pr 6 O 11 /アルミナ上
アルミナの担体粒子を硝酸プラセオジムで少し湿らせる程度に含浸し、乾燥し、1200°Fで2時間カ焼して10%のPr6O11の濃度レベルを得る。
NO捕捉量×105 NO捕捉保持率、%
モル/g (水蒸気処理した状態のもの)
対照例 A 1.39 22
対照例 B 1.13 28
対照例 C 0.75 30
対照例 D 0.58 32
実施例 1 4.45 65
実施例 2 4.9 67
実施例 3 4.61 67
実施例 4 3.58 64
上記の説明から分かるように、本発明の範囲内にある実施例1〜4は対照例A〜Dに比べて実質的に大きなNO捕捉量およびNO捕捉保持率を与える。酸化セリウムおよび酸化プラセオジムはそれぞれ単独では殆どNO捕捉量を与えない(対照例CおよびD)という点で、この試験の結果は予想できないものである。
Claims (22)
- 流動接触分解法における触媒の再生の際NOxの放出を低減させるために炭化水素分解触媒に添加されるNOx除去組成物において、該組成物は(i)酸性酸化物担体、(ii)酸化セリウム、(iii)酸化セリウム以外のランタニド系列の元素の少なくとも1種の酸化物、および(iv)周期律表の第Ib族から選ばれる遷移金属の少なくとも1種の酸化物およびそれらの混合物を含んで成り、(ii)対(iii)の割合は重量で少なくとも1.66:1の範囲にあることを特徴とするNOx除去組成物。
- 該酸性酸化物担体はアルミナおよびシリカ−アルミナから成る群から選ばれることを特徴とする請求項1記載の組成物。
- 該酸性酸化物担体はアルミナであることを特徴とする請求項2記載の組成物。
- 該酸性酸化物担体はシリカ−アルミナであることを特徴とする請求項2記載の組成物。
- 該シリカ−アルミナはアルミナ対シリカのモル比が1:1ないし最高50:1であることを特徴とする請求項4記載の組成物。
- 該シリカ−アルミナはカ焼したカオリンからシリカを苛性浸出することによってつくられることを特徴とする請求項4記載の組成物。
- 該シリカ−アルミナはその特徴的発熱線によりカ焼したカオリンからシリカを苛性浸出することによってつくられることを特徴とする請求項4記載の組成物。
- 苛性浸出を受けたカオリン担体は微小球体であり、該苛性浸出されたカオリンはその特徴的発熱線によりカ焼する前にクロロ水酸化アルミニウムに結合していることを特徴とする請求項7記載の組成物。
- 該第Ib族の遷移金属は銅、銀およびそれらの混合物から成る群から選ばれることを特徴とする請求項1記載の組成物。
- 該酸化セリウムは該酸性酸化物担体100重量部当たり少なくとも0.5重量部の量で存在することを特徴とする請求項1記載の組成物。
- 酸化セリウム以外のランタニド系列の元素の該酸化物は酸化プラセオジムであることを特徴とする請求項1記載の組成物。
- (a)炭化水素の分解に触媒作用を及ぼすのに適した触媒組成物、および(b)(i)酸性酸化物担体、(ii)酸化セリウム、(iii)酸化セリウム以外のランタニド系列の元素の少なくとも1種の酸化物、および(iv)周期律表の第Ib族から選ばれる遷移金属の酸化物を含んで成るNOx低減用組成物を含んで成り、(ii)対(iii)の割合は重量で少なくとも1.66:1の範囲にあり,該NOx低減用組成物は該触媒組成物と一体となった成分であるか、触媒組成物粒子とは別になった粒子であるか、或いはそれらの混合物であり、そして該NOx低減用組成物は流動分解触媒組成物の0.1〜15重量%をなしていることを特徴とする流動分解触媒組成物。
- 該分解触媒は成分(a)および成分(b)の混合物を含んで成ることを特徴とする請求項12記載の分解触媒組成物。
- 該分解触媒は成分(a)および成分(b)の両方を含む一体となった粒子であることを特徴とする請求項12記載の分解触媒組成物。
- 酸化セリウム以外のランタニド系列の元素の該酸化物は酸化プラセオジムであることを特徴とする請求項12記載の分解触媒組成物。
- 炭化水素供給原料の流動接触分解を行い低分子量の成分にする際NOxの放出を低減する方法において、該方法は炭化水素供給原料を高温において炭化水素の接触分解を行うのに適した分解触媒と接触させNOx低減用組成物の存在下において低分子量の炭化水素成分を生成させ、この際該NOx低減用組成物は(i)酸性酸化物担体、(ii)酸性酸化物担体100重量部当たり少なくとも0.5重量部の酸化セリウム、(iii)酸化セリウム以外のランタニド系列の元素の少なくとも1種の酸化物、および(iv)周期律表の第Ib族から選ばれる遷移金属の酸化物を含んで成り、該NOx低減用組成物は、分解触媒の0.1〜15重量%をなしているものであり、そして(ii)対(iii)の割合は重量で少なくとも1.66:1の範囲にあることを特徴とする方法。
- 該分解触媒およびNOx低減用組成物は分解触媒成分およびそれとは別になったNOx低減用組成物成分の混合物を含んで成ることを特徴とする請求項16記載の方法。
- 該分解触媒およびNOx低減用組成物は分解触媒成分とNOx低減用組成物成分との一体となった組み合わせを含んで成ることを特徴とする請求項16記載の方法。
- 該分解触媒は炭化水素供給原料と接触する際流動化させられることを特徴とする請求項16記載の方法。
- 該接触工程から得られる使用された分解触媒を回収し、該触媒を再生する条件下において該使用した触媒を処理し、再生させる工程をさらに含むことを特徴とする請求項19記載の方法。
- 該炭化水素供給原料は少なくとも0.1重量%の窒素を含んでいることを特徴とする請求項16記載の方法。
- 酸化セリウム以外のランタニド系列の元素の該少なくとも1種の酸化物は酸化プラセオジムであることを特徴とする請求項16記載の方法。
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ES2092429B1 (es) | 1993-07-29 | 1997-08-01 | Univ Valencia Politecnica | Catalizador para la eliminacion de sox y nox de gases, especialmente de unidades fcc, y manera de prepararlo. |
US5426083A (en) | 1994-06-01 | 1995-06-20 | Amoco Corporation | Absorbent and process for removing sulfur oxides from a gaseous mixture |
US20020092795A1 (en) | 1995-05-05 | 2002-07-18 | Peters Alan W. | NOx reduction compositions for use in FCC processes |
US6165933A (en) | 1995-05-05 | 2000-12-26 | W. R. Grace & Co.-Conn. | Reduced NOx combustion promoter for use in FCC processes |
US6129834A (en) | 1995-05-05 | 2000-10-10 | W. R. Grace & Co. -Conn. | NOx reduction compositions for use in FCC processes |
US6248688B1 (en) | 1996-09-27 | 2001-06-19 | Engelhard Corporation | Catalyst composition containing oxygen storage components |
US6107240A (en) | 1997-03-26 | 2000-08-22 | Engelhard Corporation | Catalyst composition containing an intimately mixed oxide of cerium and praseodymium |
US6800586B2 (en) * | 2001-11-23 | 2004-10-05 | Engelhard Corporation | NOx reduction composition for use in FCC processes |
-
2001
- 2001-11-23 US US10/001,485 patent/US6800586B2/en not_active Expired - Lifetime
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2002
- 2002-11-05 KR KR1020047007770A patent/KR100998819B1/ko active IP Right Grant
- 2002-11-05 JP JP2003547547A patent/JP4443226B2/ja not_active Expired - Fee Related
- 2002-11-05 AU AU2002342336A patent/AU2002342336B2/en not_active Ceased
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- 2002-11-05 EP EP02776460.4A patent/EP1446462B1/en not_active Expired - Lifetime
- 2002-11-05 WO PCT/US2002/035462 patent/WO2003046112A1/en active Application Filing
- 2002-11-11 TW TW091133060A patent/TWI281875B/zh active
- 2002-11-19 MY MYPI20024316A patent/MY134248A/en unknown
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2004
- 2004-01-13 US US10/756,095 patent/US6852298B2/en not_active Expired - Lifetime
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Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JP2006503699A (ja) * | 2002-10-21 | 2006-02-02 | ダブリュー・アール・グレイス・アンド・カンパニー−コネチカット | FCC法に使用されるNOx低減組成物 |
Also Published As
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WO2003046112A1 (en) | 2003-06-05 |
US7045485B2 (en) | 2006-05-16 |
TWI281875B (en) | 2007-06-01 |
US20040141897A1 (en) | 2004-07-22 |
US6800586B2 (en) | 2004-10-05 |
US6852298B2 (en) | 2005-02-08 |
AU2002342336B2 (en) | 2008-05-29 |
MY134248A (en) | 2007-11-30 |
EP1446462B1 (en) | 2015-03-18 |
KR20040055810A (ko) | 2004-06-26 |
US20040141898A1 (en) | 2004-07-22 |
TW200300364A (en) | 2003-06-01 |
JP2005510356A (ja) | 2005-04-21 |
KR100998819B1 (ko) | 2010-12-06 |
US20030098259A1 (en) | 2003-05-29 |
AU2002342336A1 (en) | 2003-06-10 |
EP1446462A1 (en) | 2004-08-18 |
CA2468152C (en) | 2011-10-18 |
CA2468152A1 (en) | 2003-06-05 |
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