JP2022545638A - 鉄促進化ゼオライトおよびそれから作製された触媒 - Google Patents
鉄促進化ゼオライトおよびそれから作製された触媒 Download PDFInfo
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- JP2022545638A JP2022545638A JP2022508912A JP2022508912A JP2022545638A JP 2022545638 A JP2022545638 A JP 2022545638A JP 2022508912 A JP2022508912 A JP 2022508912A JP 2022508912 A JP2022508912 A JP 2022508912A JP 2022545638 A JP2022545638 A JP 2022545638A
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- iron
- zeolite
- catalyst
- promoted
- scr
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- 239000003054 catalyst Substances 0.000 title claims abstract description 201
- 239000010457 zeolite Substances 0.000 title claims abstract description 145
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims abstract description 205
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims abstract description 126
- 229910021536 Zeolite Inorganic materials 0.000 claims abstract description 125
- 239000000203 mixture Substances 0.000 claims abstract description 107
- 229910052742 iron Inorganic materials 0.000 claims abstract description 92
- 238000000034 method Methods 0.000 claims abstract description 52
- 238000010531 catalytic reduction reaction Methods 0.000 claims abstract description 12
- 239000000758 substrate Substances 0.000 claims description 97
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 claims description 48
- 238000006243 chemical reaction Methods 0.000 claims description 47
- 239000000463 material Substances 0.000 claims description 45
- 229910052751 metal Inorganic materials 0.000 claims description 42
- 239000002184 metal Substances 0.000 claims description 42
- 239000007789 gas Substances 0.000 claims description 36
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 29
- 230000008569 process Effects 0.000 claims description 16
- 238000000576 coating method Methods 0.000 claims description 15
- 229910021529 ammonia Inorganic materials 0.000 claims description 13
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 11
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 10
- 239000011248 coating agent Substances 0.000 claims description 10
- 238000005342 ion exchange Methods 0.000 claims description 8
- 239000012530 fluid Substances 0.000 claims description 6
- 239000000377 silicon dioxide Substances 0.000 claims description 6
- 230000032683 aging Effects 0.000 claims description 5
- 239000000919 ceramic Substances 0.000 claims description 4
- 230000003647 oxidation Effects 0.000 claims description 4
- 238000007254 oxidation reaction Methods 0.000 claims description 4
- 238000004891 communication Methods 0.000 claims description 2
- 239000002002 slurry Substances 0.000 description 36
- 239000002808 molecular sieve Substances 0.000 description 34
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 34
- 239000010410 layer Substances 0.000 description 27
- 230000003197 catalytic effect Effects 0.000 description 25
- 230000000052 comparative effect Effects 0.000 description 18
- 238000011068 loading method Methods 0.000 description 15
- 239000011148 porous material Substances 0.000 description 15
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 description 13
- 150000002739 metals Chemical class 0.000 description 13
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 12
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 10
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 10
- 239000004202 carbamide Substances 0.000 description 9
- 229910052782 aluminium Inorganic materials 0.000 description 8
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 7
- 238000001035 drying Methods 0.000 description 7
- 239000007787 solid Substances 0.000 description 7
- 239000004071 soot Substances 0.000 description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 7
- DUFCMRCMPHIFTR-UHFFFAOYSA-N 5-(dimethylsulfamoyl)-2-methylfuran-3-carboxylic acid Chemical compound CN(C)S(=O)(=O)C1=CC(C(O)=O)=C(C)O1 DUFCMRCMPHIFTR-UHFFFAOYSA-N 0.000 description 6
- 230000015572 biosynthetic process Effects 0.000 description 6
- 238000001354 calcination Methods 0.000 description 6
- 239000003638 chemical reducing agent Substances 0.000 description 6
- 239000010949 copper Substances 0.000 description 6
- 239000010936 titanium Substances 0.000 description 6
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 5
- 229910045601 alloy Inorganic materials 0.000 description 5
- 239000000956 alloy Substances 0.000 description 5
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 5
- 229910000323 aluminium silicate Inorganic materials 0.000 description 5
- 229910052802 copper Inorganic materials 0.000 description 5
- 238000000227 grinding Methods 0.000 description 5
- 229930195733 hydrocarbon Natural products 0.000 description 5
- 150000002430 hydrocarbons Chemical class 0.000 description 5
- 238000002156 mixing Methods 0.000 description 5
- 229910052757 nitrogen Inorganic materials 0.000 description 5
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 4
- 229910002091 carbon monoxide Inorganic materials 0.000 description 4
- 150000001768 cations Chemical class 0.000 description 4
- 239000011651 chromium Substances 0.000 description 4
- 229910052760 oxygen Inorganic materials 0.000 description 4
- -1 oxygen ion Chemical class 0.000 description 4
- 229910052710 silicon Inorganic materials 0.000 description 4
- 229910052719 titanium Inorganic materials 0.000 description 4
- 238000011144 upstream manufacturing Methods 0.000 description 4
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 3
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 3
- 238000007792 addition Methods 0.000 description 3
- 238000003915 air pollution Methods 0.000 description 3
- 229910052783 alkali metal Inorganic materials 0.000 description 3
- 150000001340 alkali metals Chemical class 0.000 description 3
- 239000012298 atmosphere Substances 0.000 description 3
- 229910052804 chromium Inorganic materials 0.000 description 3
- 239000011247 coating layer Substances 0.000 description 3
- 229910052878 cordierite Inorganic materials 0.000 description 3
- 239000002178 crystalline material Substances 0.000 description 3
- 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 3
- MVFCKEFYUDZOCX-UHFFFAOYSA-N iron(2+);dinitrate Chemical compound [Fe+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MVFCKEFYUDZOCX-UHFFFAOYSA-N 0.000 description 3
- 239000011572 manganese Substances 0.000 description 3
- 229910052759 nickel Inorganic materials 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 230000009467 reduction Effects 0.000 description 3
- 238000011946 reduction process Methods 0.000 description 3
- 238000006722 reduction reaction Methods 0.000 description 3
- 229910052718 tin Inorganic materials 0.000 description 3
- 229910052726 zirconium Inorganic materials 0.000 description 3
- 229910000505 Al2TiO5 Inorganic materials 0.000 description 2
- 229910017119 AlPO Inorganic materials 0.000 description 2
- 241000269350 Anura Species 0.000 description 2
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 2
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 2
- GQPLMRYTRLFLPF-UHFFFAOYSA-N Nitrous Oxide Chemical compound [O-][N+]#N GQPLMRYTRLFLPF-UHFFFAOYSA-N 0.000 description 2
- 229910052581 Si3N4 Inorganic materials 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
- 125000000129 anionic group Chemical group 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 229910052796 boron Inorganic materials 0.000 description 2
- 229910010293 ceramic material Inorganic materials 0.000 description 2
- 238000002485 combustion reaction Methods 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
- 239000006260 foam Substances 0.000 description 2
- 229910052733 gallium Inorganic materials 0.000 description 2
- 229910052732 germanium Inorganic materials 0.000 description 2
- 229910052738 indium Inorganic materials 0.000 description 2
- 239000004615 ingredient Substances 0.000 description 2
- 229910052748 manganese Inorganic materials 0.000 description 2
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 229910001092 metal group alloy Inorganic materials 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 229910052863 mullite Inorganic materials 0.000 description 2
- 239000010955 niobium Substances 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 239000013618 particulate matter Substances 0.000 description 2
- 230000035515 penetration Effects 0.000 description 2
- 239000002243 precursor Substances 0.000 description 2
- AABBHSMFGKYLKE-SNAWJCMRSA-N propan-2-yl (e)-but-2-enoate Chemical compound C\C=C\C(=O)OC(C)C AABBHSMFGKYLKE-SNAWJCMRSA-N 0.000 description 2
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 2
- 229910010271 silicon carbide Inorganic materials 0.000 description 2
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 2
- 229910052845 zircon Inorganic materials 0.000 description 2
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 description 2
- GHOKWGTUZJEAQD-ZETCQYMHSA-N (D)-(+)-Pantothenic acid Chemical compound OCC(C)(C)[C@@H](O)C(=O)NCCC(O)=O GHOKWGTUZJEAQD-ZETCQYMHSA-N 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- 229910052684 Cerium Inorganic materials 0.000 description 1
- 229910001200 Ferrotitanium Inorganic materials 0.000 description 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 1
- 229910002651 NO3 Inorganic materials 0.000 description 1
- 229910052779 Neodymium Inorganic materials 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- XOJVVFBFDXDTEG-UHFFFAOYSA-N Norphytane Natural products CC(C)CCCC(C)CCCC(C)CCCC(C)C XOJVVFBFDXDTEG-UHFFFAOYSA-N 0.000 description 1
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 1
- 240000007594 Oryza sativa Species 0.000 description 1
- 235000007164 Oryza sativa Nutrition 0.000 description 1
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 1
- 229910052777 Praseodymium Inorganic materials 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 1
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 1
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- 150000001255 actinides Chemical class 0.000 description 1
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- 229910052784 alkaline earth metal Inorganic materials 0.000 description 1
- 150000001342 alkaline earth metals Chemical class 0.000 description 1
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical group [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 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
- CNLWCVNCHLKFHK-UHFFFAOYSA-N aluminum;lithium;dioxido(oxo)silane Chemical compound [Li+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O CNLWCVNCHLKFHK-UHFFFAOYSA-N 0.000 description 1
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- 125000002091 cationic group Chemical group 0.000 description 1
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- 230000001413 cellular effect Effects 0.000 description 1
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
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- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
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- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
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- 238000010438 heat treatment Methods 0.000 description 1
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- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 description 1
- PVFSDGKDKFSOTB-UHFFFAOYSA-K iron(3+);triacetate Chemical compound [Fe+3].CC([O-])=O.CC([O-])=O.CC([O-])=O PVFSDGKDKFSOTB-UHFFFAOYSA-K 0.000 description 1
- 229910052747 lanthanoid Inorganic materials 0.000 description 1
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- 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
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- 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
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- ZSDSQXJSNMTJDA-UHFFFAOYSA-N trifluralin Chemical compound CCCN(CCC)C1=C([N+]([O-])=O)C=C(C(F)(F)F)C=C1[N+]([O-])=O ZSDSQXJSNMTJDA-UHFFFAOYSA-N 0.000 description 1
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- WTHDKMILWLGDKL-UHFFFAOYSA-N urea;hydrate Chemical compound O.NC(N)=O WTHDKMILWLGDKL-UHFFFAOYSA-N 0.000 description 1
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- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
Images
Classifications
-
- 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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/30—Ion-exchange
-
- 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
- B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
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Abstract
【選択図】図5
Description
本出願は、2019年8月29日に出願された、米国仮出願第62/893,543号全体に対する優先権の利益を主張するものである。
4NO+4NH3+O2→4N2+6H2O(標準のSCR反応)
2NO2+4NH3+O2→3N2+6H2O(遅いSCR反応)
NO+NO2+2NH3→2N2+3H2O(高速SCR反応)
本明細書に開示される触媒組成物は、一般に、例えば鉄促進モレキュラーシーブの総重量に基づいて、少なくとも約6重量パーセントの鉄を含む鉄促進モレキュラーシーブを含み、モレキュラーシーブの鉄含有量が、少なくとも2つの別々のステップでモレキュラーシーブに添加された、選択的触媒還元(SCR)触媒組成物を含む。本明細書で使用される場合に「モレキュラーシーブ」という表現は、ゼオライトおよび他の骨格材料(例えば、同形置換された材料)などの骨格材料を指し、これらは、例えば、粒子形態で、1つ以上の促進剤金属と組み合わせて、触媒として使用され得る。モレキュラーシーブは、一般的に四面体型の部位を含み、かつ実質的に均一な細孔分布を有し、平均細孔径が20Å以下の、広範な三次元網目構造の酸素イオンに基づく材料である。細孔径は環径により定義される。本明細書で使用される場合、「ゼオライト」という用語は、ケイ素およびアルミニウム原子をさらに含むモレキュラーシーブの具体的な例を指している。1つ以上の実施形態によれば、モレキュラーシーブをそれらの構造型によって定義することは、その構造型を有するモレキュラーシーブと、同じ構造型を有するSAPO、AlPOおよびMeAPO材料などのありとあらゆるアイソタイプ骨格材料との両方を含むことを意図することが理解されよう。
1つ以上の実施形態によれば、基材(開示された触媒組成物が触媒物品、例えば、SCR触媒物品を得るために適用される)は、自動車触媒を調製するために典型的に使用される任意の材料から構築され得、典型的には金属またはセラミックのハニカム構造で構成される。本明細書で使用される場合、「基材」という用語は、触媒材料が典型的にはウォッシュコートの形態で適用されるモノリス材料を指す。基材は、典型的には、SCRウォッシュコート組成物(例えば、本明細書で上に開示された金属促進化モレキュラーシーブを含む)が適用および接着される複数の壁面を提供し、それによって触媒組成物の担体として作用する。1つ以上の実施形態では、基材は、フロースルーハニカムモノリスまたは微粒子フィルターのうちの1つ以上から選択され、触媒材料は、ウォッシュコートとして基材に適用される。
本開示によれば、SCR触媒組成物は、一般に、第1の金属促進化モレキュラーシーブ材料を提供することによって調製される。上記のように、本開示の様々な実施形態において、第1の金属促進化モレキュラーシーブ材料は、テンプレート不使用の合成法によって調製された低シリカ-アルミナ鉄促進化ベータゼオライトであり得る。他の種類のモレキュラーシーブを調製する方法は、当技術分野で知られており、開示された組成物内に含めるための所望のゼオライト骨格を提供するために容易に使用することができる。ゼオライトは、ゼオライト構造内にすでに第1の鉄含有量が存在する状態で調製するか、または初期の鉄含有量を確立するために以下に記載されるように処理することができる。
上で言及したように、触媒組成物は、調製され、基材上にコーティングされる。この方法は、本明細書に概して開示される触媒組成物(または触媒組成物の1つ以上の成分)を溶媒(例えば、水)と混合して、触媒基材をコーティングするためのスラリーを形成することを含むことができる。本明細書に記載の第2の金属含有量で促進された金属促進化ゼオライト材料を含む触媒組成物は、スラリーの形態で調製することができる。
得られる触媒物品(基材上の1つ以上のウォッシュコート層を含み、触媒組成物でコーティングされた基材を提供する)は、様々な構成を有することができる。いくつかの実施形態では、本明細書で言及したように、開示される触媒組成物のすべての成分(第2の金属含有量成分を有する金属促進化ゼオライトを含む)は、単一の触媒組成物ウォッシュコート層(すなわち、混合物)内に含有され、これは基材上の1つ以上の層として提供される。いくつかの実施形態では、基材上にコーティングされた触媒組成物が別個のウォッシュコート層を含み、少なくとも1つのウォッシュコート層が本明細書に記載の金属促進化ゼオライトを含み、少なくとも1つの(別個の)ウォッシュコート層が本明細書による第2の金属含有量を有する金属促進化ゼオライト成分を含まない、触媒物品が提供される。この実施形態では、他のウォッシュコート層は、PGM、具体的にはPtを含有し得、本開示の金属促進化ゼオライトと一緒にした場合、選択的アンモニア酸化触媒(AMOx)として機能する。
本開示による触媒組成物を利用する窒素酸化物の選択的還元は、一般に、アンモニアまたは尿素の存在下で実施される。特に、本明細書に記載の方法に従って調製された触媒組成物を含むSCRシステムは、車両の排気ガス処理システムに統合することができる。例示的なSCRシステムは、以下の成分を含むことができる。本明細書に記載のSCR触媒組成物、尿素貯蔵タンク、尿素ポンプ、尿素投与システム、尿素インジェクター/ノズル、およびそれぞれの制御ユニット。
本発明の態様は、以下の実施例によってさらに完全に例示され、これらは、本発明のある特定の態様を記載するために例示されるのであって、本発明を限定するものとして解釈されるべきではない。
40のシリカ-アルミナ比および1.4重量%のFe2O3充填量を有する従来のFe促進化ベータ触媒組成物を使用して、固形分が約40%のSCR触媒スラリーを調製した。このスラリーに、か焼された触媒上に5重量%のZrO2を提供するように設計されたレベルで酢酸ジルコニウムを添加した。この参照触媒を、400セル/平方インチ(cpsi)のセル密度および6ミルの壁厚を有するセル状セラミックモノリス上にウォッシュコートした。直径1インチ×長さ3インチのモノリスサンプルをコーティングし、110℃で乾燥させた後、450℃で1時間か焼した。ウォッシュコート、乾燥、およびか焼を繰り返して3.0g/in3のウォッシュコート充填量を達成した。
本開示による第2の鉄含有量を有するFe促進化ベータ触媒組成物を調製した。
スラリー内イオン交換プロセスを使用して、第1のゼオライト材料に追加の鉄を添加し、第2の鉄含有量を有する第2のFe促進化低SARベータゼオライト(サンプルCおよびDに使用)を形成した。本開示による第2のFe促進化低SARベータゼオライトは、Fe2O3として計算して、ゼオライト材料の総重量に基づいて、約6.6重量%の第2の鉄含有量を有していた。
本開示による第2の鉄含有量を有するFe促進化ベータ触媒組成物を調製した。
スラリー内イオン交換プロセスを使用して、ゼオライト材料に追加の鉄を添加し、本開示による第2の鉄含有量を有する第2のFe促進化低SARベータゼオライト(サンプルGおよびHに使用)を形成した。第2のFe促進化低SARベータゼオライトは、Fe2O3として計算して、ゼオライト材料の総重量に基づいて、約8.5重量%の第2の鉄含有量を有していた。
上記の実施例1に従って調製された、第2のFe促進化低SARベータゼオライト触媒組成物を含むSCR触媒物品のサンプルCおよびDを、deNOx性能について評価した。比較目的のために、第1のFe促進化低SARベータゼオライト触媒組成物を含むSCR触媒物品のサンプルAおよびBを、上記の比較例1に従って調製し、これらもdeNOx性能について評価した。記載されたように基材上に触媒スラリーをウォッシュコートすることによって、SCRサンプルを調製した。
上記の実施例2に従って調製された、第2のFe促進化低SARベータゼオライト触媒組成物を含むSCR触媒物品のサンプルGおよびHを、deNOx性能について評価した。比較目的のために、第1のFe促進化低SARベータゼオライト触媒組成物を含むSCR触媒物品のサンプルEおよびFを、上記の比較例2に従って調製し、これらもdeNOx性能について評価した。記載されたように基材上に触媒スラリーをウォッシュコートすることによって、SCRサンプルを調製した。
実施例1(6.6重量%の総Fe2O3充填量を有する二重Fe交換)のデータを、比較例2(7.4重量%のFe2O3充填量を有する単一Fe交換)のデータと比較した。
Claims (18)
- 選択的触媒還元(SCR)触媒を形成する方法であって、
第1の鉄含有量を有する第1の鉄促進化ゼオライトを受け取ることと、
イオン交換ステップにおいて前記鉄促進化ゼオライトを追加の鉄で処理して、第2の鉄含有量を有する第2の鉄促進化ゼオライトを形成することと、を含み、前記第2の鉄含有量は、前記第1の鉄含有量よりも高い、方法。 - 前記鉄促進化ゼオライトの総重量に基づいて、前記第1の鉄含有量が約2~約8重量%であり、前記第2の鉄含有量が約6~約10重量%である、請求項1に記載の方法。
- 前記第2の鉄含有量が、前記第1の鉄含有量よりも少なくとも約15%高く、より具体的には少なくとも約20%高い、請求項1に記載の方法。
- 前記鉄促進化ゼオライトが、BEA骨格構造を有するゼオライト材料である、請求項1に記載の方法。
- 前記BEA骨格構造を有するゼオライト材料が、有機テンプレート不使用の合成プロセスから得られる、請求項4に記載の方法。
- 前記鉄促進化ゼオライトが、約10以下のシリカ対アルミナモル比(SAR)を有する、請求項1に記載の方法。
- 前記鉄促進化ゼオライトが、約5以下のシリカ対アルミナモル比(SAR)を有する、請求項1に記載の方法。
- 前記触媒が、イオン交換鉄と、前記触媒の水熱エージング後に窒素酸化物を含有する排気流中で前記触媒のNOx転化性能を維持するのに十分な量の非交換鉄と、を含有する、請求項1に記載の方法。
- 前記第2の鉄含有量を有する第2の鉄促進化ゼオライトの新鮮なサンプルが、250°Cの温度で、前記第1の鉄促進化ゼオライトの新鮮なサンプルよりも少なくとも約15%高いNOx転化率、より具体的には少なくとも約20%または25%または30%または35%または40%高いNOx転化率を有する、請求項1に記載の方法。
- フロースルーセラミックまたは金属基材を前記第2の鉄促進化ゼオライトでコーティングすることによってSCR触媒物品を調製することをさらに含む、先行請求項のいずれか一項に記載の方法。
- 多孔性壁流フィルター基材をさらに含む、先行請求項のいずれか一項に記載の方法。
- 先行請求項のいずれか一項に記載の方法に従って作製された鉄促進化ゼオライト。
- 選択的触媒還元(SCR)触媒組成物であって、約10未満のSARを有する鉄促進化低SARベータゼオライトを含み、前記鉄促進化ゼオライトの総重量に基づいて少なくとも約6重量パーセントの鉄を含み、前記ベータゼオライトの鉄含有量が、少なくとも2つの別々のステップで前記ゼオライトに添加された、SCR触媒組成物。
- 前記触媒組成物が、フロースルーまたは壁流フィルター基材上に配置される、請求項13に記載のSCR触媒組成物。
- エンジン排気ガス処理システムであって、先行請求項のいずれか一項に従って作製された触媒組成物と、リーンバーンエンジンと流体連通している排気ガス導管と、を含み、前記触媒組成物が、前記排気ガス導管の下流にある、エンジン排気ガス処理システム。
- 前記エンジンが、ディーゼルエンジンである、請求項15に記載のエンジン排気ガス処理システム。
- 低SCRのFe促進化ベータゼオライトSCR触媒の前に、DOCおよび/またはCSF触媒があり、かつ追加のCu-ゼオライトSCR触媒および/または選択的アンモニア酸化触媒(AMOx)が続いてもよく、前記Cu-ゼオライトSCR触媒およびAMOx触媒が、Cu-CHAを含む、請求項15に記載のエンジン排気ガス処理システム。
- リーンバーンエンジンからの排気ガスから窒素酸化物を除去する方法であって、リーンバーンエンジンからの排気ガス流を、先行請求項のいずれか一項に従って調製された触媒組成物と接触させることを含む、方法。
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