CN106457146B - 区域化催化剂复合材料 - Google Patents
区域化催化剂复合材料 Download PDFInfo
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- CN106457146B CN106457146B CN201580032197.XA CN201580032197A CN106457146B CN 106457146 B CN106457146 B CN 106457146B CN 201580032197 A CN201580032197 A CN 201580032197A CN 106457146 B CN106457146 B CN 106457146B
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- catalyst composite
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- washcoat
- zoned catalyst
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- 239000003054 catalyst Substances 0.000 title claims abstract description 96
- 239000002131 composite material Substances 0.000 title claims description 65
- 230000003197 catalytic effect Effects 0.000 claims abstract description 40
- 239000000463 material Substances 0.000 claims abstract description 36
- 238000000034 method Methods 0.000 claims abstract description 15
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 claims description 24
- 239000007789 gas Substances 0.000 claims description 22
- 229910052751 metal Inorganic materials 0.000 claims description 22
- 239000002184 metal Substances 0.000 claims description 22
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 22
- 239000002562 thickening agent Substances 0.000 claims description 19
- 239000002245 particle Substances 0.000 claims description 18
- 239000004094 surface-active agent Substances 0.000 claims description 16
- 239000010953 base metal Substances 0.000 claims description 15
- 239000002270 dispersing agent Substances 0.000 claims description 15
- 150000001875 compounds 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
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical group [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 12
- 229910002091 carbon monoxide Inorganic materials 0.000 claims description 12
- 238000002485 combustion reaction Methods 0.000 claims description 12
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 11
- 229910052760 oxygen Inorganic materials 0.000 claims description 11
- 239000001301 oxygen Substances 0.000 claims description 11
- 238000003860 storage Methods 0.000 claims description 11
- 239000012530 fluid Substances 0.000 claims description 10
- 239000002808 molecular sieve Substances 0.000 claims description 10
- 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 10
- 239000004071 soot Substances 0.000 claims description 9
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 8
- 229910021529 ammonia Inorganic materials 0.000 claims description 4
- 238000000399 optical microscopy Methods 0.000 claims description 4
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 claims description 3
- 238000004891 communication Methods 0.000 claims description 3
- 229910000037 hydrogen sulfide Inorganic materials 0.000 claims description 3
- 238000004519 manufacturing process Methods 0.000 claims description 3
- 238000003963 x-ray microscopy Methods 0.000 claims description 3
- 239000000758 substrate Substances 0.000 abstract description 35
- 239000002002 slurry Substances 0.000 description 28
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 26
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 15
- 238000011068 loading method Methods 0.000 description 11
- 229910052763 palladium Inorganic materials 0.000 description 11
- 229910052697 platinum Inorganic materials 0.000 description 9
- 230000003647 oxidation Effects 0.000 description 8
- 238000007254 oxidation reaction Methods 0.000 description 8
- 238000002360 preparation method Methods 0.000 description 8
- 239000006254 rheological additive Substances 0.000 description 8
- 239000007787 solid Substances 0.000 description 8
- 230000000052 comparative effect Effects 0.000 description 7
- 229910044991 metal oxide Inorganic materials 0.000 description 7
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- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 6
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 6
- 239000000203 mixture Substances 0.000 description 6
- 230000004584 weight gain Effects 0.000 description 6
- 235000019786 weight gain Nutrition 0.000 description 6
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- 239000000956 alloy Substances 0.000 description 5
- 238000001354 calcination Methods 0.000 description 5
- 229910000420 cerium oxide Inorganic materials 0.000 description 5
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 5
- 238000009826 distribution Methods 0.000 description 5
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 5
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 5
- 239000011148 porous material Substances 0.000 description 5
- -1 Platinum Group Metals Chemical class 0.000 description 4
- 229910021536 Zeolite Inorganic materials 0.000 description 4
- 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 4
- 150000002739 metals Chemical class 0.000 description 4
- 239000003870 refractory metal Substances 0.000 description 4
- 238000004626 scanning electron microscopy Methods 0.000 description 4
- 239000003381 stabilizer Substances 0.000 description 4
- 229910052712 strontium Inorganic materials 0.000 description 4
- 238000012360 testing method Methods 0.000 description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
- OFOBLEOULBTSOW-UHFFFAOYSA-N Malonic acid Chemical compound OC(=O)CC(O)=O OFOBLEOULBTSOW-UHFFFAOYSA-N 0.000 description 3
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 description 3
- 229910052782 aluminium Inorganic materials 0.000 description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 3
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- 238000006243 chemical reaction Methods 0.000 description 3
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 3
- 239000011248 coating agent Substances 0.000 description 3
- 238000000576 coating method Methods 0.000 description 3
- 238000013461 design Methods 0.000 description 3
- 238000007598 dipping method Methods 0.000 description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 3
- 239000007788 liquid Substances 0.000 description 3
- 239000002609 medium Substances 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
- VZCYOOQTPOCHFL-OWOJBTEDSA-N Fumaric acid Chemical compound OC(=O)\C=C\C(O)=O VZCYOOQTPOCHFL-OWOJBTEDSA-N 0.000 description 2
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 2
- 229910052779 Neodymium Inorganic materials 0.000 description 2
- 229910018879 Pt—Pd Inorganic materials 0.000 description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- WNLRTRBMVRJNCN-UHFFFAOYSA-N adipic acid Chemical compound OC(=O)CCCCC(O)=O WNLRTRBMVRJNCN-UHFFFAOYSA-N 0.000 description 2
- 239000004411 aluminium Substances 0.000 description 2
- 229910000323 aluminium silicate Inorganic materials 0.000 description 2
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 238000010531 catalytic reduction reaction Methods 0.000 description 2
- 229910052804 chromium Inorganic materials 0.000 description 2
- 239000011651 chromium Substances 0.000 description 2
- 239000003426 co-catalyst Substances 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 229910052878 cordierite Inorganic materials 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
- XBDQKXXYIPTUBI-UHFFFAOYSA-N dimethylselenoniopropionate Natural products CCC(O)=O XBDQKXXYIPTUBI-UHFFFAOYSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 230000002209 hydrophobic effect Effects 0.000 description 2
- 238000009616 inductively coupled plasma Methods 0.000 description 2
- 229910052742 iron Inorganic materials 0.000 description 2
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 description 2
- 229910052749 magnesium Inorganic materials 0.000 description 2
- 239000011777 magnesium Substances 0.000 description 2
- 229910052748 manganese Inorganic materials 0.000 description 2
- 239000011572 manganese Substances 0.000 description 2
- 229910001092 metal group alloy Inorganic materials 0.000 description 2
- 150000007522 mineralic acids Chemical class 0.000 description 2
- QEFYFXOXNSNQGX-UHFFFAOYSA-N neodymium atom Chemical compound [Nd] QEFYFXOXNSNQGX-UHFFFAOYSA-N 0.000 description 2
- 150000007524 organic acids Chemical class 0.000 description 2
- 150000002894 organic compounds Chemical class 0.000 description 2
- XNGIFLGASWRNHJ-UHFFFAOYSA-N phthalic acid Chemical compound OC(=O)C1=CC=CC=C1C(O)=O XNGIFLGASWRNHJ-UHFFFAOYSA-N 0.000 description 2
- 229910052761 rare earth metal Inorganic materials 0.000 description 2
- 150000002910 rare earth metals Chemical class 0.000 description 2
- 239000010948 rhodium Substances 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 2
- 239000010936 titanium Substances 0.000 description 2
- VZCYOOQTPOCHFL-UHFFFAOYSA-N trans-butenedioic acid Natural products OC(=O)C=CC(O)=O VZCYOOQTPOCHFL-UHFFFAOYSA-N 0.000 description 2
- 229910052720 vanadium Inorganic materials 0.000 description 2
- 239000013598 vector Substances 0.000 description 2
- RTBFRGCFXZNCOE-UHFFFAOYSA-N 1-methylsulfonylpiperidin-4-one Chemical compound CS(=O)(=O)N1CCC(=O)CC1 RTBFRGCFXZNCOE-UHFFFAOYSA-N 0.000 description 1
- 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 1
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229910001200 Ferrotitanium Inorganic materials 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 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
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 1
- 229910052777 Praseodymium Inorganic materials 0.000 description 1
- 229910052581 Si3N4 Inorganic materials 0.000 description 1
- KDYFGRWQOYBRFD-UHFFFAOYSA-N Succinic acid Natural products OC(=O)CCC(O)=O KDYFGRWQOYBRFD-UHFFFAOYSA-N 0.000 description 1
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- 238000005054 agglomeration Methods 0.000 description 1
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- 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
- 238000004458 analytical method Methods 0.000 description 1
- JFCQEDHGNNZCLN-UHFFFAOYSA-N anhydrous glutaric acid Natural products OC(=O)CCCC(O)=O JFCQEDHGNNZCLN-UHFFFAOYSA-N 0.000 description 1
- 239000012736 aqueous medium Substances 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- ITHZDDVSAWDQPZ-UHFFFAOYSA-L barium acetate Chemical compound [Ba+2].CC([O-])=O.CC([O-])=O ITHZDDVSAWDQPZ-UHFFFAOYSA-L 0.000 description 1
- TZCXTZWJZNENPQ-UHFFFAOYSA-L barium sulfate Inorganic materials [Ba+2].[O-]S([O-])(=O)=O TZCXTZWJZNENPQ-UHFFFAOYSA-L 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910052797 bismuth Inorganic materials 0.000 description 1
- KDYFGRWQOYBRFD-NUQCWPJISA-N butanedioic acid Chemical compound O[14C](=O)CC[14C](O)=O KDYFGRWQOYBRFD-NUQCWPJISA-N 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
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- 150000001768 cations Chemical class 0.000 description 1
- 239000001913 cellulose Substances 0.000 description 1
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- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 1
- RCFVMJKOEJFGTM-UHFFFAOYSA-N cerium zirconium Chemical compound [Zr].[Ce] RCFVMJKOEJFGTM-UHFFFAOYSA-N 0.000 description 1
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- 238000012512 characterization method Methods 0.000 description 1
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- 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
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- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- FYDKNKUEBJQCCN-UHFFFAOYSA-N lanthanum(3+);trinitrate Chemical compound [La+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O FYDKNKUEBJQCCN-UHFFFAOYSA-N 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
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- VZCYOOQTPOCHFL-UPHRSURJSA-N maleic acid Chemical compound OC(=O)\C=C/C(O)=O VZCYOOQTPOCHFL-UPHRSURJSA-N 0.000 description 1
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- 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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- 238000012856 packing Methods 0.000 description 1
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- PUDIUYLPXJFUGB-UHFFFAOYSA-N praseodymium atom Chemical compound [Pr] PUDIUYLPXJFUGB-UHFFFAOYSA-N 0.000 description 1
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- IUVKMZGDUIUOCP-BTNSXGMBSA-N quinbolone Chemical compound O([C@H]1CC[C@H]2[C@H]3[C@@H]([C@]4(C=CC(=O)C=C4CC3)C)CC[C@@]21C)C1=CCCC1 IUVKMZGDUIUOCP-BTNSXGMBSA-N 0.000 description 1
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- 229910052703 rhodium Inorganic materials 0.000 description 1
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
- VXNYVYJABGOSBX-UHFFFAOYSA-N rhodium(3+);trinitrate Chemical compound [Rh+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VXNYVYJABGOSBX-UHFFFAOYSA-N 0.000 description 1
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- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 1
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- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 1
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- 238000004611 spectroscopical analysis Methods 0.000 description 1
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- 239000010935 stainless steel Substances 0.000 description 1
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Abstract
本发明提供区域化催化剂,其能在较短区域内有效地利用组分以实现转化和/或捕捉在废气流中的一种或多种组分的特定功能。高度受控的区域化是从整料载体的一端形成的。这些区域具有平面形状以使在基材的每个通道内的区域化催化材料是处于与载体一端之间基本上均匀的距离。也提供了制备和使用所述区域化催化剂的方法。
Description
发明领域
本发明涉及废气纯化催化剂及其使用方法。更具体而言,本发明涉及区域化催化剂复合材料,其包含在整料载体上的催化材料区域,其中此区域具有所需的功能,例如快速点火和/或烟灰燃烧。所述区域具有平面形状,使得在基材的每个通道内的区域化催化材料处于与载体一端之间基本上均匀的距离。这些区域提供催化活性、捕捉组分和/或吸附组分的性能。这些区域提供沿着区域长度的基本上均匀的厚度和组分浓度。
发明背景
催化转化器用于处理燃烧发动机的废气流,从而转化、捕捉和/或吸附不需要的组分以满足严格的排放标准。在催化转化器中使用的组分包括、但不限于铂族金属(PGM)、基础金属(BM)、储氧组分(OSC)和/或分子筛,例如沸石。催化转化器被设计成满足具体应用的需要,例如用于柴油发动机的废气流(例如柴油氧化催化剂(DOC)、选择性催化还原(SCR)催化剂和催化烟灰过滤剂(CSF))和汽油发动机的废气流(三效转化(TWC)催化剂)。进一步设计区域化和/或层状催化剂以实现在特定位置的特定化学作用。
美国专利No.7,189,376(Kumar)公开了多区域化催化剂及其捕捉应用。美国专利No.7,749,472(Chen)提供了一种罩面涂层以提供抗中毒催化剂。
本领域仍然需要区域化催化制品,其能提供优异的催化活性、组分的捕捉和/或吸附性能。
发明概述
本发明提供改进的区域化催化剂,其能在较短区域内有效地利用组分以实现特定的功能。高度受控的区域是从整料载体的一端形成的。这些区域具有平面形状以使在基材的每个通道内的区域化催化材料处于与载体一端之间基本上均匀的距离。
第一方面提供一种用于内燃机废气流的区域化催化剂复合材料,其包含:含有多个纵向通道的整料载体;从载体一端开始的区域,并且此区域沿着纵向通道进行轴向延伸以使得此区域具有平面形状,此区域含有能转化和/或捕捉在废气流中的一种或多种组分的催化材料。
所述组分可以是一氧化碳(CO),烃(HC),氮氧化物(NOx),烟灰,氨(NH3),SOx(SO2,SO3)和/或硫化氢(H2S)。此区域可以占载体长度的至多1英寸(2.54cm)。此区域可以占载体长度的2mm至0.5英寸(1.27cm)。此区域可以具有10-60μm的平均厚度。此区域可以从载体涂料形成,所述载体涂料是剪切变稀的并具有在5-7范围内的假塑性指数。此区域可以从粘度为100-750厘泊(cp)的载体涂料形成的。此区域可以从屈服点为1.5-10.0的载体涂料形成。此区域可以从负载量为0.10-1.0g/in3的载体涂料形成。
催化材料可以含有铂族金属(PGM)、基础金属(BM)、储氧组分(OSC)和/或分子筛。此区域可以具有5-20μm的平均粒径。
所述区域可以从含有催化材料以及流变体系的载体涂料形成,所述流变体系具有包含聚合物增稠剂、表面活性剂和/或分散剂的一种或多种化合物。流变体系含有聚合物增稠剂、表面活性剂和分散剂。
从所述区域到载体一端的距离可以在通道至通道之间距离的0-15%(相对)的范围内变化。在载体一端处的区域的催化材料中的活性组分浓度与在所述区域结束处的浓度相比可以在不大于10%的量的范围内变化。在载体一端处的每个通道的区域厚度与在所述区域结束处的厚度相比可以在不大于15%的量的范围内变化。
本发明的另一个方面提供一种用于处理包含烃、一氧化碳和其它废气组分的内燃机废气流的体系,此排放处理体系包含:排气管道,其经由排气歧管与内燃机以流体方式连通;和本发明所述的任何一种区域化催化剂复合材料。
本发明的另一个方面提供一种处理废气的方法,包括使得含有烃、一氧化碳和氮氧化物的气态料流与本发明所述的任何一种区域化催化剂复合材料接触。
在另一个方面中提供一种制备区域化催化剂复合材料的方法,此方法包括:形成剪切变稀载体涂料;和将包含多个纵向通道的整料载体的入口端浸渍到载体涂料中达到一定深度以形成具有平面形状的入口区域。此方法可以还包括在浸渍之后,提供经由纵向通道的气态脉冲以除去过量的载体涂料。此方法还包括在浸渍步骤期间向通道施加真空压力。
附图简述
可以考虑结合以下对于各种实施方案的详细描述以及附图更完全地理解本发明,在附图中:
图1提供区域化催化剂复合材料和非区域化催化剂复合材料的照片;
图2提供具有平面形状的区域化催化剂复合材料的特写照片;
图3提供非平面的区域形状的照片;
图4提供示例性的区域化催化剂复合材料的显微照片;
图5和6提供示例性区域化催化剂复合材料的基于线扫描的组分含量的照片;和
图7提供在区域化催化剂复合材料和非区域化催化剂复合材料之间的压降的图。
详细描述
发现使用具有剪切变稀粘度性能的载体涂料允许从整料载体的一端形成高度受控的区域,从而可以浓缩活性组分例如铂族金属(PGM)、基础金属(BM)、储氧组分(OSC)和/或分子筛,以用于点火和/或烟灰燃烧和/或捕捉目的。
术语“整料载体”表示单一结构,其是均匀和连续的,并且不是通过将单独的载体小块固定在一起形成的。
“区域”是(直接或间接地)位于基材上的催化材料,其处于从基材的一端开始的基材部分上。“入口区域”表示这种区域是从基材的入口端开始,并且在沿着基材向下朝向出口端的轴向距离处结束,但是延伸的距离小于基材的整个距离,其中入口端是废气首先进入的那个末端。“出口区域”表示这种区域是从基材的出口端开始,并且在沿着基材向上朝向入口端的轴向距离处结束,但是延伸的距离小于基材的整个距离,其中出口端是废气排出的那个末端。短的区域是优选的,例如至多1英寸(2.54cm)或甚至0.5英寸(1.27cm)或甚至0.25英寸(0.63cm)。区域化催化剂复合材料可以具有入口区域、出口区域,或同时具有入口区域和出口区域。每个区域可以设计成用于满足具体应用的特定功能。
“高度受控”表示由于载体涂料在整料载体的通道中的均匀分布,此区域具有平面形状。因此,“平面形状”是指具有基本上均匀厚度的催化材料,其中催化材料与载体一端之间的距离也是基本上均匀的。例如,通道至通道的距离可以在此距离的0-5%的小范围内变化,这通过数字X-射线或光学显微术检测。另外,区域的厚度可以仅仅在不大于15%的范围内变化,这通过光学或扫描电子显微术(SEM)检测。也可以预期的是,在区域内的成分的浓度是基本上均匀的。例如,对于每个通道,在载体一端处的区域的催化材料中的活性成分浓度与在沿着通道距离在所述区域结束处的浓度相比是在不大于10%的范围内变化,这是通过电感耦合等离子体光谱(ICP)检测的。为了获得平面形状,载体涂料是从催化材料和流变改性剂体系形成的,其中流变改性剂体系是一种或多种有机化合物,其包含聚合物增稠剂、表面活性剂和/或分散剂,用于改进载体涂料的流变性能。
这里使用的术语“载体涂料”具有在本领域中的常规含义,即施用到载体上的催化材料或其它材料的薄的粘附性涂料。
这里使用的术语“剪切变稀”表示流体的粘度在施加剪切应力时降低。假塑性指数是描绘流体的剪切变稀特性的一个参数,其定义为在6rpm时的粘度/在60rpm时的粘度之间的无量纲比率。另一种表示剪切变稀特性的参数是流体的屈服点,其中屈服点是流体开始发生不可逆/塑性的变形时的应力。参见Herschel-Bulkley流变模型,屈服点定义为τ0,流动指数n定义粘度类型,τ0>0且n<1表示假塑性(剪切变稀行为)。优选的τ0范围是1.5-10.0,n的范围是0.5-0.9(都是无单位的)。
这里使用的术语“平均粒径”表示粒径密度(分布),其中d50表示平均粒径或作为分布的50%规定的尺寸,d10、d90和d99进一步限定分布宽度,其中窄分布是优选的。这些检测是基于使用Cilas 1090双重激光粒径分析仪,其能检测尺寸在0.04-500mm范围内的粒子,所有检测是基于从湿分散体、即浆液(粒子在含水介质中的混合物,固体比例为10-50重量%)取得的样品。
在载体涂料中的“空隙”或“大孔”表示不含能通过扫描电子显微术(SEM)且在最宽部分处分辨的物质的区域。
区域化催化剂复合材料和催化材料
区域化催化剂复合材料是如下制备的:形成剪切变稀载体涂料,其被设计成满足所述区域的所需功能;并将整料载体的一端浸渍到载体涂料中达到一定深度以形成沿着载体的纵向通道具有平面形状的区域。可以向这些通道施加真空以促进通道被载体涂料涂覆。气态脉冲可以经由通道沿着与浸渍端面相反的方向施加,从而除去任何过量的载体涂料和随后保持平面形状。一般而言,区域是施用在位于整料载体上的下层催化剂复合材料上。或者,如果需要的话,区域可以直接施用到载体上。
作为在下层催化剂复合材料上的区域的一个例子,为了改进三效转化(TWC)催化剂或柴油氧化催化剂(DOC)的点火,例如可以将含有钯的入口区域施用到已经设计用于满足TWC或DOC功能的催化剂复合材料上。相对于下层催化剂复合材料,额外贵金属组分在区域中的存在能促进点火。作为另一个例子,选择性催化还原(SCR)催化剂复合材料可以通过加入包含额外沸石和/或基础金属的出口区域来改进,其能转化残余的氨(NH3)。在DOC上,另一个例子是包含分子筛的入口区域,分子筛可以用于改进在冷启动期间的烃捕捉性能。对于烟灰和SOF(可溶性有机级分),可以加入额外PGM和/或基础金属的短区域以氧化过量的烟灰和SOF,从而防止聚集、随后的压降增加以及DOC和任何额外组分在排气体系下游结焦(例如SCR催化剂)。在另一个例子中,短区域包含高度浓缩的Ni、Mn、Sr和Ce氧化物以结合和/或捕捉硫化合物,从而在更受控的<750℃的低温条件下释放/再生。这尤其对于含有Ba的催化剂而言是有益的,因为BaSO4通常需要较高的>850℃的再生温度。
适合于区域的催化材料包括、但不限于:铂族金属(PGM),基础金属(BM),储氧组分(OSC),和/或分子筛。载体涂料是通过催化材料和流变改性剂体系的浆液形成的。
应当理解的是,用于特定区域中的材料能彼此相容,并能有效地实现所需功能。
合适的PGM可以包括:钯,铑,铂,和/或它们的组合。
合适的基础金属可以包括:Ni,Fe,Mn,Cu,Co,Ba,Mg,Ga,Ca,Sr,V,W,Bi和/或Mo。
合适的储氧组分可以包括:氧化铈,氧化镨,或它们的组合。氧化铈向区域中的输送可以通过使用例如以下物质实现:氧化铈,铈和锆的混合氧化物,和/或铈、锆和钕的混合氧化物。
分子筛表示具有基本上均匀的孔分布的材料,其中平均孔径是不大于沸石是具有较均匀的孔径的硅铝酸盐结晶材料,其中根据沸石的类型以及在沸石晶格中所含阳离子的类型和含量,孔直径通常是约3-10埃。具体的非限定性例子包括SSZ-13,SSZ-62,Beta(β)。SAPO型分子筛表示角共享四面体框架,其中大部分的四面体位置被铝和磷占据。SAPO型分子筛的非限定性例子包括硅铝磷酸盐和ALPO型金属-铝磷酸盐。一个具体的非限定性例子包括SAPO-34。
所述区域是较短的,并且可以占载体长度的至多1英寸(2.54cm)。在一个具体例子中,这些区域占载体长度的2mm至0.5英寸(1.27cm)的范围。这些区域可以从负载量为0.10-1.0g/in3或0.20-0.8g/in3或甚至0.40-0.6g/in3的载体涂料形成。关于厚度,区域通常具有10-60μm的平均厚度。区域可以含有5-20μm的平均粒径。应当注意的是,对于一个或多个实施方案,粒径范围是窄的,在5-20μm的载体涂料中也产生相似的无规空隙(大孔)。
通过本文所述的技术尽可能减少了区域的可变性。例如,从通道至通道的距离可以在0-5%的小范围内变化(或0.5-4%或1-3%)。另外,厚度可以仅仅变化不大于15%(或10%或甚至5%)。另外,对于每个通道,活性组分的浓度可以变化不大于10%(或7.5或甚至5%),这通过SEM检测。
示例性的涂覆器包含:用于载体涂料的储库;以及浸渍组件,其包括臂,与臂连接操作的夹子,以及控制器,从而在将基材固定在夹子中之后,浸渍组件将整料载体的包含多个纵向通道的入口端浸渍到储库中达到一定深度;或辊压台,其用于将浸渍载体涂料或另一种载体涂料施用到基材的表面上。载体涂料通常具有剪切变稀性能。连接至涂覆器的气体源可以在浸渍组件或辊压台步骤之后提供经由纵向通道的气态脉冲。涂覆器可以还包含煅烧组件,其用于向区域化催化复合材料赋予热量。载体所浸渍的深度是基于在长度、厚度和/或干增重方面的区域设计确定的。如此形成的区域化催化复合材料具有入口区域,后者具有平面形状。参见图1,具有平面形状20的区域化催化剂复合材料10是如实施例2所述在下层催化剂上使用流变体系制备的。非区域化催化剂复合材料12如图1中的对比例3所示,其仅仅具有下层催化剂,并不具有区域。图2证明了具有平面形状的短区域,其公称长度是0.5”(12.7mm),是如实施例5所述制备的。
在图3中提供现有技术实施例的照片,其中在不存在流变改性剂体系的情况下制备区域,从而证明其是曲折的,或不是平面形状的,并且不具有本发明实施方案中的平面形状。
流变体系
用于区域的载体涂料是从催化材料与流变改性剂和/或改性剂混合物形成的。流变改性剂是由能向具有特定固体负载量的载体涂料赋予粘度和剪切变稀性能的化合物构成的,并且也抑制载体涂料在基材通道中的毛细作用。示例性的剪切变稀特性可以是在5-7范围内的假塑性指数。载体涂料的示例性粘度可以在100-750厘泊(cP)的范围内。载体涂料的示例性屈服点可以在1.5-10.0的范围内。
流变改性剂可以具有例如一种或多种有机化合物,其包含聚合物增稠剂、表面活性剂和/或分散剂。这种组合将在本文中称为流变体系。特定实施方案包括所有组分:聚合物增稠剂、表面活性剂和分散剂。示例性的聚合物增稠剂是缔合增稠剂,但是其它常规增稠剂可以是合适的,例如纤维素。用于本文流变体系中的增稠剂通常是疏水性的。表面活性剂优选具有低的HLB(亲水亲油平衡值),例如在2-6的范围内,这有利于与疏水性材料之间的相容性。分散剂能帮助在载体涂料中的材料很好地分布或分散,这同时包括有机和无机材料。具有全部聚合物增稠剂、低HLB表面活性剂和分散剂的流变体系提供各功能的协同组合以提供剪切变稀载体涂料。在煅烧催化剂复合材料时,流变体系的各组分被除去,产生与大孔之间的一些附加互联(较小的孔),大孔主要通过无机载体涂料组分的颗粒填充密度形成。
下层催化剂复合材料
下层催化剂复合材料可以通过本领域公知的方法制备。一种代表性方法如下所述。按照需要,下层催化剂复合材料可以在载体上作为多层制备。对于由载体涂料形成的任何层,高表面积耐火金属氧化物例如γ-氧化铝的细分散粒子在合适的介质例如水中淤浆化。在一个或多个实施方案中,浆液是酸性的,具有约2至小于约7的pH。浆液的pH可以通过向浆液加入足量的无机酸或有机酸来降低。当考虑酸和原料的相容性时,可以使用两者的组合。无机酸包括、但不限于硝酸。有机酸包括、但不限于:乙酸,丙酸,草酸,丙二酸,琥珀酸,戊二酸,己二酸,马来酸,富马酸,邻苯二甲酸,酒石酸,柠檬酸等等。然后,如果需要的话,可以向浆液加入储氧组分的水溶性或水分散性化合物,例如铈-锆复合材料,稳定剂,例如乙酸钡,以及助催化剂,例如硝酸镧。然后可以将浆液粉碎得到基本上全部的具有粒径小于约20微米的固体,即平均直径为约0.1-15微米。粉碎可以在球磨机或其它相似设备中完成,并且浆液的固含量可以例如是约10-50重量%,更特别是约10-40重量%。然后可以将载体在这种浆液中浸渍一次或多次,或可以将浆液涂覆到载体上,从而在载体上沉积具有所需负载量的载体涂料/金属氧化物复合材料,例如约0.5-3.0g/in3。
然后,经涂覆的载体通过加热进行煅烧,例如在500-600℃煅烧约1-3小时。通常,当需要钯时,钯组分是以化合物或复合物的形式使用,以实现此组分在耐火金属氧化物载体、例如活化氧化铝上的分散。在本发明中,术语“钯组分”表示任何化合物、复合物等等,其在煅烧或使用时分解或转化成催化活性形式,通常是金属或金属氧化物。可以使用金属组分的水溶性化合物或者水分散性化合物或复合物,只要用于将金属组分浸渍或沉积到耐火金属氧化物载体粒子上的液体介质不会不利地与金属或其化合物或其复合物或在催化剂组合物中可能存在的其它组分反应即可,并且液体介质能通过在加热和/或施加真空时挥发或分解而从金属组分除去。在一些情况下,可以不进行液体的去除操作,直至将催化剂投入使用和经受在操作期间遇到的高温。一般而言,从经济和环境方面考虑,使用贵金属的可溶性化合物或复合物的水溶液。例如,合适的化合物是硝酸钯或硝酸铑。在煅烧步骤期间,或至少在使用复合材料的初始阶段期间,这些化合物被转化成金属或其化合物的催化活性形式。
可以按照与上文关于在载体上沉积任何层所述相同的方式在第一层上制备和沉积额外层。
催化层也可以按照需要含有稳定剂和助催化剂。合适的稳定剂包括一种或多种不可还原的金属氧化物,其中金属是选自钡、钙、镁、锶和它们的混合物。优选,稳定剂含有钡和/或锶的一种或多种氧化物。合适的助催化剂包括选自以下的一种或多种稀土金属的一种或多种不可还原的氧化物:镧,镨,钇,锆和它们的混合物。
催化层也可以含有储氧组分。通常,储氧组分将含有一种或多种稀土金属的一种或多种可还原的氧化物。合适的储氧组分的例子包括氧化铈,氧化镨,或它们的组合。氧化铈向层中的输送可以通过使用例如以下物质完成:氧化铈,铈和锆的混合氧化物,和/或铈、锆和钕的混合氧化物。
载体
在一个或多个实施方案中,催化材料位于载体上。载体可以是通常用于制备催化剂复合材料的任何材料,并优选含有陶瓷或金属蜂窝结构。可以使用任何合适的载体,例如具有从基材入口端面或出口端面延伸的多个精细平行气流通道的整料基材,使得这些通道对于从中流过的流体是开放的(在本文中称为蜂窝流通型基材)。从其流体入口到其流体出口形成基本直线路径的那些通道被壁限定,在所述壁上,催化材料作为载体涂料涂覆,以使得从这些通道流过的气体与催化材料接触。整料基材的流动通道是薄壁型通道,其可以具有任何合适的横截面形状和尺寸,例如梯形、长方形、正方形、正弦形、六边形、椭圆形、圆形等。这些结构可以含有约60-900或更多个气体入口开口(即小室)/每平方英寸横截面。
载体也可以是壁流动型过滤剂基材,其中通道是另外封闭的,允许气态料流从一个方向进入通道(入口方向),经由通道壁流动,并从另一个方向从通道出来(出口方向)。双重氧化催化剂组合物可以涂覆在壁流动过滤剂上。如果使用这种载体,则所得体系将能除去颗粒物质以及气态污染物。壁流动型过滤剂载体可以由本领域公知的材料制成,例如堇青石或碳化硅。
载体可以由任何合适的耐火材料制成,例如堇青石,堇青石-氧化铝,氮化硅,锆莫来石,锂辉石,氧化铝-氧化硅氧化镁,硅酸锆,硅线石,硅酸镁,锆,透锂长石,氧化铝,硅铝酸盐等等。
用于本发明催化剂的载体也可以是金属性质的,并由一种或多种金属或金属合金组成。金属载体可以按照各种不同的形状使用,例如波纹片或整料形式。优选的金属载体包括耐热性金属和金属合金,例如钛和不锈钢,以及其中铁作为基本或主要组分的其它合金。这些合金可以含有镍、铬和/或铝中的一种或多种,并且这些金属的总量可以有利地是合金的至少15重量%,例如10-25重量%的铬、3-8重量%的铝和至多20重量%的镍。合金也可以含有少量或痕量的一种或多种其它金属,例如锰、铜、钒、钛等等。金属载体的表面可以在高温下氧化,例如1000℃和更高的温度,从而通过在载体表面上形成氧化物层来改进合金的耐腐蚀性。这种高温引起的氧化可以改进耐火金属氧化物载体和催化促进金属组分对载体的附着性。
在其它实施方案中,一种或多种催化剂组合物可以沉积在开孔泡沫基材上。这些基材是本领域公知的,通常由耐火陶瓷或金属材料形成。
在描述本发明的多个示例性实施方案之前,应当理解的是,本发明不限于在以下描述中给出的结构或工艺步骤的细节。本发明能具有其它实施方案和按照不同方式实施。在下文中,提供关于混合金属氧化物复合材料的优选设计,包括所述单独特征的组合或无限制的组合及其应用,包括本发明其它方面的催化剂、体系和方法。
在实施方案1中,一种用于内燃机废气流的区域化催化剂复合材料包含:含有多个纵向通道的整料载体;从载体一端开始的区域,此区域沿着纵向通道进行轴向延伸以使得此区域具有平面形状,此区域含有能转化和/或捕捉在废气流中的一种或多种组分的催化材料。
在实施方案2中,提供一种用于处理包含烃、一氧化碳和其它废气组分的内燃机废气流的体系,此排放处理体系包含:排气管道,其经由排气歧管与内燃机以流体方式连通;和本文所述的任何一种区域化催化剂复合材料。
在实施方案3中,提供一种处理废气的方法,包括使得含有烃、一氧化碳和氮氧化物的气态料流与本文所述的任何一种区域化催化剂复合材料接触。
在实施方案4中,提供一种制备区域化催化剂复合材料的方法,包括:形成剪切变稀载体涂料;和将包含多个纵向通道的整料载体的入口端浸渍到载体涂料中达到一定深度以形成具有平面形状的入口区域。
实施方案1-4中的任何一个可以具有一个或多个以下任选的设计特征:
所述组分是一氧化碳(CO),烃(HC),氮氧化物(NOx),烟灰,氨(NH3),SOx(SO2,SO3)和/或硫化氢(H2S);
所述区域占载体长度的至多1英寸(2.54cm);
所述区域占载体长度的2mm至0.5英寸(1.27cm);
所述区域具有10-60μm的平均厚度;
所述区域是从载体涂料形成的,此载体涂料具有假塑性指数为5-7的剪切变稀性能;
所述区域是从粘度为100-750厘泊(cp)的载体涂料形成的;
所述区域是从屈服点为1.5-10.0的载体涂料形成的;
所述区域是从负载量为0.10-1.0g/in3的载体涂料形成的;
催化材料含有铂族金属(PGM)、基础金属(BM)、储氧组分(OSC)和/或分子筛;
所述区域具有5-20μm的平均粒径;
所述区域是从含有催化材料以及流变体系的载体涂料形成的,所述流变体系具有包含聚合物增稠剂、表面活性剂和/或分散剂的一种或多种化合物;
流变体系含有聚合物增稠剂、表面活性剂和分散剂;
从所述区域到载体一端的距离是在通道至通道之间距离的0-15%的范围内变化;
在载体一端处的区域的催化材料中的活性组分浓度与在所述区域结束处的浓度相比是在不大于10%的量的范围内变化;
在载体一端处的每个通道的区域厚度与在所述区域结束处的厚度相比是在不大于15%的量的范围内变化;
在浸渍之后,提供经由纵向通道的气态脉冲以除去过量的载体涂料;和
在浸渍步骤期间向通道施加真空压力。
实施例
以下实施例说明本发明代表性实施方案的制备和表征。但是,本发明不限于这些实施例。
实施例1
此实施例描述制备具有1英寸点火区域的区域化催化剂复合材料。通过混合氧化铝、乙酸锆和铂盐、并将pH调节到约5来制备浆液。浆液具有约43%的固含量。将浆液研磨到最终粒径为9-11微米。为了形成载体涂料,向浆液加入流变体系,其含有基于浆液重量计的0.5%分散剂、1%表面活性剂和5%的聚合物增稠剂。将流通型载体3.66”3.0”400/4(400个小室/平方英寸,具有4密耳的壁)的一端浸入载体涂料中,并施加真空以涂覆载体的通道。经涂覆的载体在连续带式煅烧器中在450℃的峰值温度下煅烧,在峰值温度下煅烧20分钟以形成短的1英寸区域化催化剂复合材料,其具有平面形状和0.55g/in3的催化材料含量干增重,和按重量计含有91.2%的氧化铝、4.6%的锆和4.2%的铂。
实施例2
此实施例描述制备在下层柴油氧化催化剂(DOC)上具有0.5英寸Pt-Pd点火区域的区域化催化剂复合材料。使用单位体积为75.44in3的3英寸基材。
在下层DOC中的各组分是高表面积的被二氧化硅掺杂的γ-氧化铝,硫酸沥滤型("SAL")β沸石,6%Pd掺杂的γ-氧化铝,氧化锆,以及铂,它们的浓度分别是基于催化剂煅烧重量计的约78.1%、12.2%、7.6%、0.83%和1.22%。在制备DOC载体涂料期间,将各组分与聚合物增稠剂和表面活性剂混合。在涂覆基材之后没有进行煅烧步骤。下层催化剂层的总负载量是3.0g/in3。DOC含有80g/ft3Pt和40g/ft3Pd。
对于入口区域,通过在被6%Pd掺杂的γ-氧化铝上负载铂来制备浆液。浆液具有约43%的固含量。将浆液研磨到最终粒径为8-10微米。为了形成载体涂料,向浆液加入流变体系,其含有基于浆液重量计的0.25%分散剂、1%表面活性剂和15%的聚合物增稠剂。将基材的一端浸入载体涂料中,并施加真空以涂覆基材的通道,然后在连续带式煅烧器中在450℃的峰值温度下煅烧,在峰值温度下煅烧20分钟以形成短的区域化催化剂复合材料,其具有平面形状并覆盖DOC催化剂。此区域具有1.0g/in3的干增重,和按重量计含有80.6%的氧化铝、9.7%的钯和9.7%的铂。
实施例3
对比
此实施例描述制备仅仅具有如实施例2中所述的下层柴油氧化催化剂(DOC)的对比例。使用单位体积为75.44in3的3英寸基材。
实施例4
测试
图1显示实施例2和对比例3的照片,其中显示实施例3的平面区域20。检测实施例2和对比例3在2英寸和3英寸的空气流下的压降。如表1所示,具有1g/in3干增重的0.5英寸区域的存在对压降没有显著影响。
表1
图4提供实施例2的区域化催化剂复合材料的末端扫描电子显微术(SEM)显微照片,其中显示入口端14,其中下层DOC催化剂16位于载体22上,区域18位于下层DOC催化剂16上。出口端24不具有区域,下层DOC催化剂16是位于载体22上。图5和6提供了实施例2的区域化催化剂复合材料的线扫描。表1证明了与非区域化催化剂复合材料的情况相比,包含高度浓缩的PGM“Ad区域(AdZone)”对于最终催化剂的流动性能、例如压降(△P)基本上没有不利影响。SEM显微照片证明薄、但均匀的罩面涂覆,并且电子探针微区分析(EPMA)线扫描显示与非区域化面积相比,PGM(同时Pd和Pt)的浓度增加5倍。
实施例5
此实施例描述制备在下层区域化三效转化(TWC)催化剂上具有0.5英寸Pd点火区域或“Ad区域”的区域化催化剂复合材料。使用600/4.3流通型基材(600个小室/平方英寸,具有4.3密耳的壁)。
下层区域化TWC催化剂具有前面的下层催化区域,其中在1.25英寸的公称距离上使用67.5g/ft3Pd,并具有0.5g/in3的干增重;和背面的下层催化区域,其中在1.25英寸的公称距离上使用12.5g/ft3Pd,并具有1.8g/in3的干增重。
在干增重为0.44g/in3的下层区域化DOC上形成300g/ft3Pd入口区域。浆液具有约11%的固含量。为了形成载体涂料,向浆液加入流变体系,其含有基于浆液重量计的0.25%分散剂、1.0%表面活性剂和15%的聚合物增稠剂。将基材的一端浸入载体涂料中,并施加真空以涂覆基材的通道,然后在连续带式煅烧器中在450℃的峰值温度下煅烧,在峰值温度下煅烧20分钟以形成短的区域化催化剂复合材料,其具有平面形状并覆盖区域化DOC催化剂。图2证明了所得的短区域具有平面形状,公称长度为0.5”(12.7mm),其中沿着纵向通道的变化是不大于12.5%。
将含有2.5g/ft3Rh和0.5g/in3干增重的顶涂层施涂到整个前面区域上,并按照2.0g/in3施涂到背面区域上。进行此操作以通过限制热量来改进短点火Pd区域的快速点火特性。
实施例6
此实施例描述制备在下层的双涂层柴油氧化催化剂(DOC)上具有0.5英寸Pt-Pd点火区域的区域化催化剂复合材料。使用两种不同的载体:Big Bore-11.8”x 4.0”Emitec300/600LS,其具有曼特尔悬垂部分(mantel overhang);和V8-7.5”x 4.0”Emitec 300/600LS,其具有曼特尔悬垂部分。
在下层DOC的底涂层中的各组分是高表面积γ-氧化铝,氧化锆,以及粘合剂,它们的浓度分别是基于催化剂煅烧重量计的约96.9%、1.2%和和1.9%。基材用底涂层载体涂料进行涂覆并煅烧。底涂层的干负载量是0.8g/in3。在下层DOC的顶涂层中的各组分是高表面积γ-氧化铝,氧化镧促进的高表面积γ-氧化铝,氧化锆,粘合剂,铂以及钯,它们的浓度分别是基于催化剂煅烧重量计的约46.95%,46.95%,2.9%,1.9%,1.1%,和0.2%。基材用顶涂层载体涂料进行涂覆并煅烧。顶涂层的干负载量是2.1g/in3。DOC含有39.2g/ft3Pt和9.8g/ft3Pd。
对于入口区域,按照实施例2所述,通过在被6%Pd掺杂的γ-氧化铝上负载铂来制备浆液。浆液具有约43%的固含量。将浆液研磨到最终粒径为8-10微米。为了形成载体涂料,向浆液加入流变体系,其含有基于浆液重量计的0.25%分散剂、1%表面活性剂和15%的聚合物增稠剂。将基材的一端浸入载体涂料中,并施加真空以涂覆基材的通道,然后在连续带式煅烧器中在450℃的峰值温度下煅烧,在峰值温度下煅烧20分钟以形成短的区域化催化剂复合材料,其具有平面形状并覆盖DOC催化剂。此区域具有1.0g/in3的干增重,和按重量计含有80.6%的氧化铝、9.7%的钯和9.7%的铂。
实施例7
对比
此实施例描述制备对比例,其仅仅具有在实施例6中所述的下层的双涂层柴油氧化催化剂(DOC)。使用两种不同的载体:Big Bore-11.8”x 4.0”Emitec 300/600LS,其具有曼特尔悬垂部分;和V8-7.5”x 4.0”Emitec300/600LS,其具有曼特尔悬垂部分。
实施例8
测试
图7显示实施例6的本发明区域复合材料(“具有0.5”Ad区域”)和对比例7的材料(“不具有Ad区域”)的压降随时间变化的图。如图7所示,具有1g/in3干增重的0.5英寸区域的存在使得能在65小时内保持压降不大于0.7inHg(英寸汞柱)。相比之下,对比例显示在小于10小时的时间内,压力增加约1.7inHg。
使用0.5英寸Ad区域能有效地保持减少的烟灰负载量和低压降(△P)。
在本说明书中提到的“一个实施方案”、“特定实施方案”、“一个或多个实施方案”或“一种实施方案”表示在至少一个本发明实施方案中包括与此实施方案相关描述的具体的特征、结构、材料或特性。因此,在说明书中各处出现的用语例如“在一个或多个实施方案中”、“在特定实施方案中”、“在一个实施方案中”或“在一种实施方案中”不是必须指代相同的本发明实施方案。另外,具体的特征、结构、材料或特性可以在一个或多个实施方案中按照任何合适的方式组合。
虽然本文中已经参照优选实施方案描述本发明,但是对于本领域技术人员显而易见的是,可以在本发明的优选设备和方法方面进行变化,而且本发明可以按照与所述不同的方式实施。因此,本发明包括属于由所附权利要求定义的本发明精神和范围内的所有修改。
Claims (13)
1.一种用于内燃机废气流的区域化催化剂复合材料,其包含:
含有多个纵向通道的整料载体;
从载体一端开始的区域,此区域沿着纵向通道进行轴向延伸以使得此区域具有平面形状,此区域含有能转化和/或捕捉在废气流中的一种或多种组分的催化材料,
其中满足至少一个以下条件:(i)通过数字X-射线或光学显微术检测,从所述区域到载体一端的距离是在通道至通道之间距离的0-15%的范围内变化;和(ii)在载体一端处的每个通道的区域厚度与在所述区域结束处的厚度相比在不大于15%的量的范围内变化;
其中所述区域占载体长度的至多1英寸(2.54cm)。
2.权利要求1的区域化催化剂复合材料,其中所述组分是一氧化碳(CO),烃(HC),氮氧化物(NOx),烟灰,氨(NH3),SOx(SO2,SO3)和/或硫化氢(H2S)。
3.权利要求1的区域化催化剂复合材料,其中所述区域占载体长度的2mm至1.27cm。
4.权利要求1的区域化催化剂复合材料,其中催化材料含有铂族金属(PGM)、基础金属(BM)、储氧组分(OSC)和/或分子筛。
5.权利要求1的区域化催化剂复合材料,其中所述区域具有10-60μm的平均厚度。
6.权利要求1的区域化催化剂复合材料,其中所述区域是从粘度为100-750厘泊(cp)的载体涂料形成的。
7.权利要求1的区域化催化剂复合材料,其中所述区域是从屈服点为1.5-10.0的载体涂料形成的。
8.权利要求1的区域化催化剂复合材料,其中所述区域是从含有催化材料以及流变体系的载体涂料形成的,所述流变体系具有包含聚合物增稠剂、表面活性剂和/或分散剂的一种或多种化合物。
9.权利要求8的区域化催化剂复合材料,其中流变体系含有聚合物增稠剂、表面活性剂和分散剂。
10.权利要求1的区域化催化剂复合材料,其中所述区域具有5-20μm的平均粒径。
11.一种用于处理包含烃、一氧化碳和其它废气组分的内燃机废气流的体系,此排放处理体系包含:
排气管道,其经由排气歧管与内燃机以流体方式连通;和
根据权利要求1的区域化催化剂复合材料。
12.一种处理废气的方法,包括使得含有烃、一氧化碳和氮氧化物的气态料流与根据权利要求1的区域化催化剂复合材料接触。
13.一种制备区域化催化剂复合材料的方法,此方法包括:
形成剪切变稀载体涂料;和将包含多个纵向通道的整料载体的入口端浸渍到载体涂料中达到一定深度以形成具有平面形状的入口区域,
其中满足至少一个以下条件:(i)通过数字X-射线或光学显微术检测,从所述区域到载体一端的距离是在通道至通道之间距离的0-15%的范围内变化;和(ii)在载体一端处的每个通道的区域厚度与在所述区域结束处的厚度相比在不大于15%的量的范围内变化;
其中所述区域占载体长度的至多1英寸(2.54cm)。
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