JP6573862B2 - 触媒化基材モノリス - Google Patents
触媒化基材モノリス Download PDFInfo
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- JP6573862B2 JP6573862B2 JP2016208575A JP2016208575A JP6573862B2 JP 6573862 B2 JP6573862 B2 JP 6573862B2 JP 2016208575 A JP2016208575 A JP 2016208575A JP 2016208575 A JP2016208575 A JP 2016208575A JP 6573862 B2 JP6573862 B2 JP 6573862B2
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- substrate monolith
- washcoat
- catalyst
- washcoat coating
- platinum
- Prior art date
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- 239000000758 substrate Substances 0.000 title claims description 156
- 230000003197 catalytic effect Effects 0.000 title description 12
- 239000003054 catalyst Substances 0.000 claims description 178
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 147
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 99
- 238000000576 coating method Methods 0.000 claims description 84
- 239000011248 coating agent Substances 0.000 claims description 79
- 239000007789 gas Substances 0.000 claims description 54
- 239000000203 mixture Substances 0.000 claims description 52
- 229910052697 platinum Inorganic materials 0.000 claims description 36
- 238000000034 method Methods 0.000 claims description 30
- 238000011144 upstream manufacturing Methods 0.000 claims description 28
- 230000003647 oxidation Effects 0.000 claims description 27
- 238000007254 oxidation reaction Methods 0.000 claims description 27
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 25
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 24
- 229910052763 palladium Inorganic materials 0.000 claims description 24
- 229910044991 metal oxide Inorganic materials 0.000 claims description 23
- 150000004706 metal oxides Chemical class 0.000 claims description 23
- 238000002485 combustion reaction Methods 0.000 claims description 19
- 238000001914 filtration Methods 0.000 claims description 19
- 229910052751 metal Inorganic materials 0.000 claims description 16
- 239000002184 metal Substances 0.000 claims description 16
- MCMNRKCIXSYSNV-UHFFFAOYSA-N ZrO2 Inorganic materials O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 15
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 claims description 15
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 claims description 15
- 239000003638 chemical reducing agent Substances 0.000 claims description 13
- 239000000463 material Substances 0.000 claims description 13
- 229910052757 nitrogen Inorganic materials 0.000 claims description 13
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 12
- 239000011959 amorphous silica alumina Substances 0.000 claims description 7
- 238000010531 catalytic reduction reaction Methods 0.000 claims description 7
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 6
- 229910052737 gold Inorganic materials 0.000 claims description 6
- 239000010931 gold Substances 0.000 claims description 6
- 238000010521 absorption reaction Methods 0.000 claims description 4
- 229910002076 stabilized zirconia Inorganic materials 0.000 claims description 4
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 3
- 229910052709 silver Inorganic materials 0.000 claims description 3
- 239000004332 silver Substances 0.000 claims description 3
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 152
- 238000006243 chemical reaction Methods 0.000 description 57
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 38
- 239000010457 zeolite Substances 0.000 description 37
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- 230000000694 effects Effects 0.000 description 31
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 26
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 26
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- 239000002808 molecular sieve Substances 0.000 description 26
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 26
- 229930195733 hydrocarbon Natural products 0.000 description 23
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- 239000010410 layer Substances 0.000 description 14
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- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 10
- 239000004202 carbamide Substances 0.000 description 10
- 239000002243 precursor Substances 0.000 description 10
- 229910052760 oxygen Inorganic materials 0.000 description 9
- NWAHZABTSDUXMJ-UHFFFAOYSA-N platinum(2+);dinitrate Chemical compound [Pt+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O NWAHZABTSDUXMJ-UHFFFAOYSA-N 0.000 description 9
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 8
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- 230000032683 aging Effects 0.000 description 7
- 229910000323 aluminium silicate Inorganic materials 0.000 description 7
- 239000012876 carrier material Substances 0.000 description 7
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- GPNDARIEYHPYAY-UHFFFAOYSA-N palladium(ii) nitrate Chemical compound [Pd+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O GPNDARIEYHPYAY-UHFFFAOYSA-N 0.000 description 7
- 238000002360 preparation method Methods 0.000 description 7
- 230000002829 reductive effect Effects 0.000 description 7
- 239000007864 aqueous solution Substances 0.000 description 6
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 6
- 239000000446 fuel Substances 0.000 description 6
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- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 4
- 229910052797 bismuth Inorganic materials 0.000 description 4
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 description 4
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- 238000011065 in-situ storage Methods 0.000 description 4
- 229910052748 manganese Inorganic materials 0.000 description 4
- 239000011572 manganese Substances 0.000 description 4
- 239000002245 particle Substances 0.000 description 4
- 239000000377 silicon dioxide Substances 0.000 description 4
- 229910052788 barium Inorganic materials 0.000 description 3
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 3
- 239000011230 binding agent Substances 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 150000002739 metals Chemical class 0.000 description 3
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- 239000013618 particulate matter Substances 0.000 description 3
- 239000006254 rheological additive Substances 0.000 description 3
- 229910052703 rhodium Inorganic materials 0.000 description 3
- 239000010948 rhodium Substances 0.000 description 3
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 3
- 238000007086 side reaction Methods 0.000 description 3
- 241000894007 species Species 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- OAKJQQAXSVQMHS-UHFFFAOYSA-N Hydrazine Chemical compound NN OAKJQQAXSVQMHS-UHFFFAOYSA-N 0.000 description 2
- -1 Platinum Group Metals Chemical class 0.000 description 2
- 229910010413 TiO 2 Inorganic materials 0.000 description 2
- 230000009471 action Effects 0.000 description 2
- 239000003463 adsorbent Substances 0.000 description 2
- 239000000956 alloy Substances 0.000 description 2
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- 239000012298 atmosphere Substances 0.000 description 2
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- 150000001875 compounds Chemical class 0.000 description 2
- 238000011109 contamination Methods 0.000 description 2
- 229910052878 cordierite Inorganic materials 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 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 2
- 238000001035 drying Methods 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 229910001657 ferrierite group Inorganic materials 0.000 description 2
- 238000009472 formulation Methods 0.000 description 2
- 206010021198 ichthyosis Diseases 0.000 description 2
- 229910052742 iron Inorganic materials 0.000 description 2
- 229910052747 lanthanoid Inorganic materials 0.000 description 2
- 150000002602 lanthanoids Chemical class 0.000 description 2
- 230000007246 mechanism Effects 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 229910052680 mordenite Inorganic materials 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 230000001737 promoting effect Effects 0.000 description 2
- 229910052761 rare earth metal Inorganic materials 0.000 description 2
- 230000001172 regenerating effect Effects 0.000 description 2
- 230000000717 retained effect Effects 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 238000003860 storage Methods 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- MGWGWNFMUOTEHG-UHFFFAOYSA-N 4-(3,5-dimethylphenyl)-1,3-thiazol-2-amine Chemical compound CC1=CC(C)=CC(C=2N=C(N)SC=2)=C1 MGWGWNFMUOTEHG-UHFFFAOYSA-N 0.000 description 1
- 229910000505 Al2TiO5 Inorganic materials 0.000 description 1
- 241000269350 Anura Species 0.000 description 1
- 229910020203 CeO Inorganic materials 0.000 description 1
- 229910052684 Cerium Inorganic materials 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 229910002651 NO3 Inorganic materials 0.000 description 1
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 1
- 230000010757 Reduction Activity Effects 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 229910052783 alkali metal Inorganic materials 0.000 description 1
- 150000001340 alkali metals Chemical class 0.000 description 1
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 1
- 150000001342 alkaline earth metals Chemical class 0.000 description 1
- JYIBXUUINYLWLR-UHFFFAOYSA-N aluminum;calcium;potassium;silicon;sodium;trihydrate Chemical compound O.O.O.[Na].[Al].[Si].[K].[Ca] JYIBXUUINYLWLR-UHFFFAOYSA-N 0.000 description 1
- BVCZEBOGSOYJJT-UHFFFAOYSA-N ammonium carbamate Chemical compound [NH4+].NC([O-])=O BVCZEBOGSOYJJT-UHFFFAOYSA-N 0.000 description 1
- 229910001423 beryllium ion Inorganic materials 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- KXDHJXZQYSOELW-UHFFFAOYSA-N carbonic acid monoamide Natural products NC(O)=O KXDHJXZQYSOELW-UHFFFAOYSA-N 0.000 description 1
- 210000004027 cell Anatomy 0.000 description 1
- 210000001175 cerebrospinal fluid Anatomy 0.000 description 1
- ZMIGMASIKSOYAM-UHFFFAOYSA-N cerium Chemical compound [Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce] ZMIGMASIKSOYAM-UHFFFAOYSA-N 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 229910001603 clinoptilolite Inorganic materials 0.000 description 1
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- 239000008367 deionised water Substances 0.000 description 1
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- 239000012467 final product Substances 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 150000004679 hydroxides Chemical class 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- 230000005764 inhibitory process Effects 0.000 description 1
- 229910001959 inorganic nitrate Inorganic materials 0.000 description 1
- ZFSLODLOARCGLH-UHFFFAOYSA-N isocyanuric acid Chemical compound OC1=NC(O)=NC(O)=N1 ZFSLODLOARCGLH-UHFFFAOYSA-N 0.000 description 1
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- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 description 1
- QGLKJKCYBOYXKC-UHFFFAOYSA-N nonaoxidotritungsten Chemical compound O=[W]1(=O)O[W](=O)(=O)O[W](=O)(=O)O1 QGLKJKCYBOYXKC-UHFFFAOYSA-N 0.000 description 1
- 230000001376 precipitating effect Effects 0.000 description 1
- 230000002265 prevention Effects 0.000 description 1
- AABBHSMFGKYLKE-SNAWJCMRSA-N propan-2-yl (e)-but-2-enoate Chemical group C\C=C\C(=O)OC(C)C AABBHSMFGKYLKE-SNAWJCMRSA-N 0.000 description 1
- 150000002910 rare earth metals Chemical class 0.000 description 1
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- 229910001930 tungsten oxide Inorganic materials 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
Images
Classifications
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- 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
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- 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
- B01D53/9409—Nitrogen oxides
- B01D53/9413—Processes characterised by a specific catalyst
- B01D53/9418—Processes characterised by a specific catalyst for removing nitrogen oxides by selective catalytic reduction [SCR] using a reducing agent in a lean exhaust gas
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- 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
- B01D53/9459—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts
- B01D53/9463—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts with catalysts positioned on one brick
- B01D53/9472—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts with catalysts positioned on one brick in different zones
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- 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
- B01D53/9459—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts
- B01D53/9477—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts with catalysts positioned on separate bricks, e.g. exhaust systems
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Description
NO+1/2O2 → NO2 (1)、及び
BaO+2NO2+1/2O2 → Ba(NO3)2 (2)
であり、ここで、反応(1)では、一酸化窒素が白金上の活性酸化部位で酸素と反応して、NO2を形成する。反応(2)は、無機硝酸塩の形の貯蔵物質によるNO2の吸着を含む。
Ba(NO3)2→BaO+2NO+3/2O2又はBa(NO3)2
→BaO+2NO2+1/2O2 (3)、及び
NO+CO→1/2N2+CO2 (4)
(他の反応には、Ba(NO3)2+8H2→BaO+2NH3+5H2O、それに続くNH3+NOx→N2+yH2O又は2NH3+2O2+CO→N2+3H2O+CO2などが含まれる。)。
4NH3+4NO+O2→4N2+6H2O(即ち、1:1 NH3:NO)(5)
4NH3+2NO+2NO2→4N2+6H2O(即ち、1:1 NH3:NOx)(6)
8NH3+6NO2→7N2+12H2O(即ち、4:3 NH3:NOx)(7)
関連がある望ましくない、非選択的な副反応は、
2NH3+2NO2→N2O+3H2O+N2 (8)
である。
4NH3+5O2→4NO+6H2O (9)
市販されているベータゼオライトを撹拌しながらFe(NO3)3の水溶液に加えた。混合した後、結合剤及びレオロジー改質剤を加えて、ウォッシュコート組成物を形成した。
脱イオン水中における比較的高い粒度分布まで粉砕したアルミナ粒子、硝酸白金、結合剤及びレオロジー改質剤の混合物を含むウォッシュコート組成物を調製した。チタン酸アルミニウムウォールフローフィルターを、出願人/譲受人の国際公開2011/080525に開示されている方法及び装置を用いてウォッシュコート添加0.2g/in3から総計Pt添加が5gft−3の触媒組成物でコーティングした。ここでは、上流側まで配向させることが意図されている第1の端部におけるチャンネルを、それらの全長の75%で、硝酸白金及び微粒子アルミナを含むウォッシュコートにより、その意図されている上流端部からコーティングし;反対端における下流側に配向させることが意図されているチャンネルを、それらの全長の25%で、入口チャンネルと同じウォッシュコートでコーティングした。すなわち、この方法は、(i)ハニカムモノリス基材を実質的に垂直に保持するステップ;(ii)基材の下端でチャンネルの開口端から所定の容量の液体を基材に導入するステップ;(iii)基材内に導入した液体を密封維持するステップ;(iv)維持した液体を含有する基材を逆にするステップと;(v)逆にした基材の下端で基材のチャンネルの開口端に減圧を施して、基材のチャンネルに沿って液体を引き込むステップを含んでいた。触媒組成物を、第1の端部からフィルターチャンネル上にコーティングし、その後コーティングしたフィルターを乾燥させた。乾燥させた第1の端部からコーティングしたフィルターを、次に回転させ、この方法を繰り返してフィルターチャンネルに同じ触媒を第2の端部からコーティングし、続いて乾燥及びか焼した。
ガス接触の入口側に向かう配向が意図されたチャンネルの全チャンネル長の100%を、硝酸白金及びアルミナを含有するウォッシュコートでコーティングしてから、コーティングしたフィルターを乾燥させ;出口側に向かって配向させることが意図されたPtコーティングしたフィルターのチャンネルの全長の35%を、硝酸パラジウム及びアルミナを含有するウォッシュコートでコーティングしたこと以外は、比較例2と同じ方法を用いて、コーティングしたフィルターを調製した。得られた完全にコーティングしたフィルターを次いで乾燥させ、次いでか焼した。コーティングしたフィルター上へのPtの完全添加量は、5gft−3であり、コーティングしたフィルター上へのPdの完全添加量は、1.75gft−3であった。
出口側に向かう配向が意図されたチャンネルの全長の35%を、アルミナのみを含有するウォッシュコートでコーティングしたこと以外は、実施例3と同じ方法を用いて、コーティングしたフィルターを調製した。得られたコーティングしたフィルターを次いで乾燥させ、次いでか焼した。コーティングしたフィルターの入口チャンネル上へのPtの完全添加量は、5gft−3であった。
フィルターの出口チャンネルに塗布したウォッシュコートが硝酸白金に加えて硝酸パラジウムを含んでいたこと以外は、比較例2と同じ方法を用いて、コーティングしたフィルターを調製した。入口及び出口チャンネルにおけるウォッシュコート添加は、入口表面と出口表面の両方の上に5g/ft3Pt、1.25g/ft3Pd添加、すなわち全PGM添加が6.25g/ft3に達するように行った。
二層のウォッシュコートを出口チャンネルの25%全ゾーン長に塗布したこと以外は、比較例2と同じ方法を用いて、コーティングしたフィルターを調製した。第1の(又は下端)層では、ウォッシュコートは、硝酸白金及びアルミナを含有していた。コーティングしたフィルターを次いで乾燥及びか焼してから、硝酸パラジウム及びアルミナを含有した第2の(又は最上)層のウォッシュコートを塗布した。入口及び出口チャンネルにおけるウォッシュコート添加は、入口チャンネル及び出口チャンネル上への全総計添加の5g/ft3Pt、1.25g/ft3Pd添加、すなわち全PGM添加が6.25g/ft3に達するように行った。
フィルターの入口チャンネルと出口チャンネルの両方に塗布したウォッシュコートが硝酸白金に加えて硝酸パラジウムを含んでいたこと以外は、比較例2と同じ方法を用いて、コーティングしたフィルターを調製した。入口及び出口チャンネルにおけるウォッシュコート添加は、入口表面と出口表面の両方の上に5g/ft3Pt、5g/ft3Pd添加、すなわち全PGM添加が10g/ft3に達するように行った。
フィルターの入口チャンネルと出口チャンネルの両方に塗布したウォッシュコートが硝酸白金に加えて硝酸パラジウムを含んでいたこと以外は、比較例2と同じ方法を用いて、コーティングしたフィルターを調製した。入口及び出口チャンネルにおけるウォッシュコート添加は、入口表面と出口表面の両方の上に5g/ft3Pt、1g/ft3Pd添加、すなわち全PGM添加が6g/ft3に達するように行った。
図1に例示されている第1の合成触媒活性試験(SCAT)実験室用反応器で試験を行った。この反応器内では、実施例1のコーティングしたFe/ベータゼオライトSCR触媒のフレッシュなコアが、比較例2又は実施例3、4、5、6、7もしくは8の触媒化ウォールフローフィルターのいずれかのコアの下流の導管に配されている。触媒行程容積が30,000hr−1で合成ガス混合物を導管に通した。フィルター入口温度900℃で60分間、定常状態の温度で触媒化ウォールフローフィルター試料を加熱(又は「エージング」)するために炉を使用し、その間、入口SCR触媒の温度は300℃であった。フィルターとSCR触媒の間の温度降下をもたらすために、空気(熱交換器)又は水冷メカニズムを使用した。エージング中のガス混合物は、10%O2、6%H2O、6%CO2、100ppmCO、400ppmNO、100ppmClとしてのHC、残余N2であった。
市販されているアルミノシリケートCHAゼオライトを、Cu(NO3)2水溶液に撹拌しながら加えた。スラリーをろ過し、次いで洗浄及び乾燥させた。所望の金属添加を達成するまで、手順を繰り返すことができる。最終生成物をか焼した。混合後、結合剤及びレオロジー改質剤を加えて、ウォッシュコート組成物を形成した。
2種のディーゼル酸化触媒を以下のように調製した:
単層DOCを以下のように調製した。硝酸白金及び硝酸パラジウムをシリカ−アルミナのスラリーに加えた。ベータゼオライトを、質量でゼオライトとして固形分の<30%を含むようにスラリーに加えた。先の実施例1の方法を用いて、ウォッシュコートスラリーを400cpsiフロースルー基材上に投与した。投与した部分を乾燥させ、次いで500℃でか焼した。ウォッシュコート被膜中の全白金族元素添加量は、60gft−3であり、全Pt:Pd重量比は4:1であった。1インチ(2.54cm)直径×3インチ(7.62cm)長のコアを完成品から切断した。得られた部品は、「フレッシュ」、すなわちエージングしていない、と表す。
単層DOCを以下のように調製した。硝酸白金及び硝酸パラジウムをシリカ−アルミナのスラリーに加えた。ベータゼオライトを、質量でゼオライトとして固形分の<30%を含むようにスラリーに加えた。DOC Aで使用したのと同じ方法を用いて、ウォッシュコートスラリーを400cpsiフロースルー基材上に投与した。投与した部分を乾燥させ、次いで500℃でか焼した。単層DOC中の全PGM添加量は、120g/ft3であり、Pt:Pd重量比は2:1であった。1インチ(2.54cm)直径×3インチ(7.62cm)長のコアを完成品から切断した。得られた部品は、「フレッシュ」、すなわちエージングしていない、と表す。
図1に例示されている第1の合成触媒活性試験(SCAT)実験室用反応器で試験を行った。この反応器内では、実施例10のコーティングしたCu/CHAゼオライトSCR触媒のエージングしたコアが、ディーゼル酸化触媒(DOC)A又はB(実施例11に基づく)のいずれかのコアの下流の導管に配されている。毎分6リットルの速度で合成ガス混合物を導管に通した。触媒出口温度900℃で2時間、定常状態の温度でDOC試料を加熱(又は「エージング」)するために炉を使用した。SCR触媒をDOC試料の下流に配置し、水冷熱交換器ジャケットも適宜使用できるが、炉の出口及びSCR入口の間のチューブの長さを調節することによってエージングプロセス中に触媒温度300℃で保持した。温度は、適切に配置した熱電対(T1及びT2)を用いて決定した。エージング中に使用したガス混合物は、40%空気、50%N2、10%H2Oであった。
全体から見て、実施例7及び8ならびに比較例2に関連して図4に示した実施例9の結果は、1:1と5:1の間のPt:Pd重量比が、触媒を含有する白金族元素から下流のSCR触媒への白金族元素、主に白金の揮発によるNOx転化活性低下の問題を低減するのに有益であることを示唆している。
Claims (15)
- 第1のウォッシュコート被膜と
第2のウォッシュコート被膜とを含み、
基材モノリスがフロースルー基材モノリスである、リーンバーン内燃機関から排出された排気ガスを処理するのに使用するための触媒化基材モノリスであって、
第1のウォッシュコート被膜は、少なくとも1種の白金族元素(PGM)と該少なくとも1種のPGMのための少なくとも1種の担体材料とを含む触媒組成物を含み、該第1のウォッシュコート被膜中の少なくとも1種のPGMは、≧700℃の温度に第1のウォッシュコート被膜を曝したときに、揮発しやすい白金を含み、
第2のウォッシュコート被膜は、第1のウォッシュコート被膜と接触した排気ガスと接触するように配向され、第2のウォッシュコート被膜が、(i)パラジウム、銀、金及びそれらの任意の2種以上の組合せからなる群から選択される金属;並びに、(ii)揮発した白金族元素(PGM)をトラップするための金属酸化物であって、該金属を担持し、且つ、安定化されていてもよいアルミナ、非晶質シリカ−アルミナ、安定化されていてもよいジルコニア、セリア、チタニア、安定化されていてもよいセリア−ジルコニア混合酸化物、及びそれらの任意の2種以上の混合物からなる群から選択される、揮発した白金族元素(PGM)をトラップするための金属酸化物;からなる触媒組成物を含む、触媒化基材モノリス。 - 第1のウォッシュコート被膜中の少なくとも1種のPGMは、白金とパラジウムの両方を含む、請求項1に記載の触媒化基材モノリス。
- Pt:Pdの重量比が≦2である、請求項2に記載の触媒化基材モノリス。
- 第2のウォッシュコート被膜は、白金及びパラジウムを含み、第2のウォッシュコート被膜中のPt:Pdの重量比が、第1のウォッシュコート被膜中のPt:Pdの重量比よりも低い、請求項1から3のいずれか一項に記載の触媒化基材モノリス。
- 第1のウォッシュコート被膜が、基材モノリスの第1のウォッシュコートゾーンに配され、第2のウォッシュコート被膜が、基材モノリスの第2のウォッシュコートゾーンに配され、第1のウォッシュコートゾーンと第2のウォッシュコートゾーンとの間に実質的に重なりがない、請求項1から4のいずれか一項に記載の触媒化基材モノリス。
- 第2のウォッシュコート被膜が、第1のウォッシュコート被膜の上の層に配されている、請求項1から4のいずれか一項に記載の触媒化基材モノリス。
- 少なくとも第1のウォッシュコート被膜が、酸化触媒又はNOx吸収触媒を含む、請求項1から6のいずれか一項に記載の触媒化基材モノリス。
- 請求項1から7のいずれか一項に記載の触媒化基材モノリスを含む、リーンバーン内燃機関のための排気システム。
- 選択接触還元(SCR)触媒を含む第2の触媒化基材モノリスを含み、第2の触媒化基材モノリスが、請求項1から7のいずれか一項に記載の触媒化基材モノリスから下流に配されている、請求項8に記載の排気システム。
- 請求項1から7のいずれか一項に記載の触媒化基材モノリスと第2の触媒化基材モノリスの間で排気ガス中に窒素還元剤を導入するための導入管を含む、請求項9に記載の排気システム。
- 第3の基材モノリスを含み、第3の基材モノリスが、フィルタリング基材モノリスであり、第3の基材モノリスが、第2の触媒化基材モノリスの下流に配されている、請求項9又は10に記載の排気システム。
- 第3の基材モノリスが酸化触媒を含む、請求項11に記載の排気システム。
- 請求項8から12のいずれか一項に記載の排気システムを含む、車両用の、リーンバーン内燃機関。
- 請求項13に記載のリーンバーン内燃機関を備えた車両。
- 白金を含む触媒組成物が、≧700℃の温度に曝されたときに、少なくとも1種の担体材料上に担持された白金を含みかつ選択接触還元(SCR)触媒の上流のフロースルー基材モノリス上に配された触媒組成物を含む第1のウォッシュコート被膜から揮発し得る白金によって、リーンバーン内燃機関の排気システム中のSCR触媒が、作用を阻害されることを低減又は防止する方法であって、揮発した白金を、第2のウォッシュコート被膜中にトラップすることを含み、第2のウォッシュコート被膜が、白金を含む触媒組成物と同じフロースルー基材モノリス上に配されかつ第1のウォッシュコート被膜と接触した排気ガスと接触するように配向され、且つ、
第2のウォッシュコート被膜が、(i)パラジウム、銀、金及びそれらの任意の2種以上の組合せからなる群から選択される金属;及び(ii)揮発した白金族元素(PGM)をトラップするための金属酸化物であって、該金属酸化物が該金属を担持し、且つ、安定化されていてもよいアルミナ、非晶質シリカ−アルミナ、安定化されていてもよいジルコニア、セリア、チタニア、安定化されていてもよいセリア−ジルコニア混合酸化物、及びそれらの任意の2種以上の混合物からなる群から選択される金属酸化物、からなる触媒組成物を含む、方法。
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Free format text: JAPANESE INTERMEDIATE CODE: R250 |
|
R250 | Receipt of annual fees |
Free format text: JAPANESE INTERMEDIATE CODE: R250 |