CN105813745B - 包含两种不同贵金属-分子筛催化剂的废气催化剂 - Google Patents
包含两种不同贵金属-分子筛催化剂的废气催化剂 Download PDFInfo
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- CN105813745B CN105813745B CN201480066490.3A CN201480066490A CN105813745B CN 105813745 B CN105813745 B CN 105813745B CN 201480066490 A CN201480066490 A CN 201480066490A CN 105813745 B CN105813745 B CN 105813745B
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- catalyst
- molecular sieve
- exhaust gas
- noble metal
- gas catalyst
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- 239000003054 catalyst Substances 0.000 title claims abstract description 250
- 239000002808 molecular sieve Substances 0.000 title claims abstract description 171
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims abstract description 173
- 229910000510 noble metal Inorganic materials 0.000 claims abstract description 40
- 238000000034 method Methods 0.000 claims abstract description 20
- 238000010521 absorption reaction Methods 0.000 claims abstract description 16
- 239000000758 substrate Substances 0.000 claims description 70
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 62
- 238000001914 filtration Methods 0.000 claims description 28
- 239000004215 Carbon black (E152) Substances 0.000 claims description 26
- 229930195733 hydrocarbon Natural products 0.000 claims description 26
- 150000002430 hydrocarbons Chemical class 0.000 claims description 26
- 229910052763 palladium Inorganic materials 0.000 claims description 24
- 239000011148 porous material Substances 0.000 claims description 18
- 239000000463 material Substances 0.000 claims description 17
- 239000003795 chemical substances by application Substances 0.000 claims description 16
- 230000003197 catalytic effect Effects 0.000 claims description 13
- 238000002485 combustion reaction Methods 0.000 claims description 13
- 238000007254 oxidation reaction Methods 0.000 claims description 10
- 230000003647 oxidation Effects 0.000 claims description 9
- 238000003795 desorption Methods 0.000 claims description 8
- 238000011144 upstream manufacturing Methods 0.000 claims description 6
- 238000010531 catalytic reduction reaction Methods 0.000 claims description 5
- 230000008859 change Effects 0.000 claims description 5
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 4
- 229910052737 gold Inorganic materials 0.000 claims description 4
- 239000010931 gold Substances 0.000 claims description 4
- GHOKWGTUZJEAQD-ZETCQYMHSA-N (D)-(+)-Pantothenic acid Chemical compound OCC(C)(C)[C@@H](O)C(=O)NCCC(O)=O GHOKWGTUZJEAQD-ZETCQYMHSA-N 0.000 claims description 3
- 239000011449 brick Substances 0.000 claims description 3
- 230000008030 elimination Effects 0.000 claims 1
- 238000003379 elimination reaction Methods 0.000 claims 1
- 238000000926 separation method Methods 0.000 claims 1
- 238000004566 IR spectroscopy Methods 0.000 abstract description 5
- 238000012545 processing Methods 0.000 abstract description 2
- 239000007789 gas Substances 0.000 description 83
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 40
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 33
- 239000011248 coating agent Substances 0.000 description 33
- 238000000576 coating method Methods 0.000 description 33
- 238000003860 storage Methods 0.000 description 28
- 229910052751 metal Inorganic materials 0.000 description 17
- 239000002184 metal Substances 0.000 description 17
- 239000002002 slurry Substances 0.000 description 16
- 229910052697 platinum Inorganic materials 0.000 description 14
- 239000000203 mixture Substances 0.000 description 13
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 11
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 9
- 239000010457 zeolite Substances 0.000 description 9
- 229910021536 Zeolite Inorganic materials 0.000 description 8
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 7
- 239000002245 particle Substances 0.000 description 7
- 239000010948 rhodium Substances 0.000 description 7
- 238000012360 testing method Methods 0.000 description 7
- 239000002585 base Substances 0.000 description 6
- 229910052802 copper Inorganic materials 0.000 description 6
- 239000010949 copper Substances 0.000 description 6
- 238000011156 evaluation Methods 0.000 description 6
- 238000001179 sorption measurement Methods 0.000 description 6
- 229910021529 ammonia Inorganic materials 0.000 description 5
- 239000012298 atmosphere Substances 0.000 description 5
- 238000001354 calcination Methods 0.000 description 5
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 5
- 229910052878 cordierite Inorganic materials 0.000 description 5
- 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 5
- 238000001125 extrusion Methods 0.000 description 5
- 238000010438 heat treatment Methods 0.000 description 5
- 238000002360 preparation method Methods 0.000 description 5
- 229910052703 rhodium Inorganic materials 0.000 description 5
- 239000002912 waste gas Substances 0.000 description 5
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 4
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 4
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 4
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 4
- 230000032683 aging Effects 0.000 description 4
- 229910000323 aluminium silicate Inorganic materials 0.000 description 4
- 239000004202 carbamide Substances 0.000 description 4
- 229910002091 carbon monoxide Inorganic materials 0.000 description 4
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 4
- 229910052742 iron Inorganic materials 0.000 description 4
- 229910052760 oxygen Inorganic materials 0.000 description 4
- 239000000843 powder Substances 0.000 description 4
- 230000008569 process Effects 0.000 description 4
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 4
- 238000006555 catalytic reaction Methods 0.000 description 3
- 238000001816 cooling Methods 0.000 description 3
- 239000003344 environmental pollutant Substances 0.000 description 3
- 238000005470 impregnation Methods 0.000 description 3
- 229910052741 iridium Inorganic materials 0.000 description 3
- 150000002739 metals Chemical class 0.000 description 3
- 238000002156 mixing Methods 0.000 description 3
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 3
- 231100000719 pollutant Toxicity 0.000 description 3
- 239000010970 precious metal Substances 0.000 description 3
- 238000006722 reduction reaction Methods 0.000 description 3
- 230000009466 transformation Effects 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 229910052684 Cerium Inorganic materials 0.000 description 2
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 229910019142 PO4 Inorganic materials 0.000 description 2
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 2
- 239000005864 Sulphur Substances 0.000 description 2
- 238000009825 accumulation Methods 0.000 description 2
- 239000000853 adhesive Substances 0.000 description 2
- 230000001070 adhesive effect Effects 0.000 description 2
- 239000003463 adsorbent Substances 0.000 description 2
- 239000004411 aluminium Substances 0.000 description 2
- 229910052782 aluminium Inorganic materials 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 229910052788 barium Inorganic materials 0.000 description 2
- 229910052791 calcium Inorganic materials 0.000 description 2
- 239000012876 carrier material Substances 0.000 description 2
- 150000001768 cations Chemical class 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- 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 2
- 235000019504 cigarettes Nutrition 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 229910052593 corundum Inorganic materials 0.000 description 2
- DIOQZVSQGTUSAI-UHFFFAOYSA-N decane Chemical compound CCCCCCCCCC DIOQZVSQGTUSAI-UHFFFAOYSA-N 0.000 description 2
- 238000007598 dipping method Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 229910052809 inorganic oxide Inorganic materials 0.000 description 2
- 238000005342 ion exchange Methods 0.000 description 2
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 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
- 229910052762 osmium Inorganic materials 0.000 description 2
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 2
- GPNDARIEYHPYAY-UHFFFAOYSA-N palladium(ii) nitrate Chemical compound [Pd+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O GPNDARIEYHPYAY-UHFFFAOYSA-N 0.000 description 2
- NWAHZABTSDUXMJ-UHFFFAOYSA-N platinum(2+);dinitrate Chemical compound [Pt+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O NWAHZABTSDUXMJ-UHFFFAOYSA-N 0.000 description 2
- 229910052700 potassium Inorganic materials 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 229910052707 ruthenium Inorganic materials 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
- 229910052709 silver Inorganic materials 0.000 description 2
- 239000004332 silver Substances 0.000 description 2
- 229910052708 sodium Inorganic materials 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 238000001228 spectrum Methods 0.000 description 2
- 239000004575 stone Substances 0.000 description 2
- 229910052712 strontium Inorganic materials 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229910052717 sulfur Inorganic materials 0.000 description 2
- 239000011593 sulfur Substances 0.000 description 2
- 239000004408 titanium dioxide Substances 0.000 description 2
- 229910001845 yogo sapphire Inorganic materials 0.000 description 2
- -1 zeolite Chemical compound 0.000 description 2
- 229910001928 zirconium oxide Inorganic materials 0.000 description 2
- 229910001017 Alperm Inorganic materials 0.000 description 1
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 1
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 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
- 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
- 229910000831 Steel Inorganic materials 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- 229910052770 Uranium Inorganic materials 0.000 description 1
- MXOSECBTSFQUJS-UHFFFAOYSA-N [O-2].[Ti+4].[V+5] Chemical compound [O-2].[Ti+4].[V+5] MXOSECBTSFQUJS-UHFFFAOYSA-N 0.000 description 1
- KTOLWOOLOCKNNB-UHFFFAOYSA-N [W+2]=O.[O-2].[Ti+4].[V+5] Chemical compound [W+2]=O.[O-2].[Ti+4].[V+5] KTOLWOOLOCKNNB-UHFFFAOYSA-N 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 239000003513 alkali Substances 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
- 150000004645 aluminates Chemical class 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
- 125000000129 anionic group Chemical group 0.000 description 1
- 239000010953 base metal Substances 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- 210000000988 bone and bone Anatomy 0.000 description 1
- 229910052792 caesium Inorganic materials 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 229910000420 cerium oxide Inorganic materials 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 239000011651 chromium Substances 0.000 description 1
- 239000003426 co-catalyst Substances 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 239000002283 diesel fuel Substances 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 239000003517 fume Substances 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 238000007654 immersion Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- 238000002329 infrared spectrum Methods 0.000 description 1
- 229910001387 inorganic aluminate Inorganic materials 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- 229910052744 lithium Inorganic materials 0.000 description 1
- HCWCAKKEBCNQJP-UHFFFAOYSA-N magnesium orthosilicate Chemical compound [Mg+2].[Mg+2].[O-][Si]([O-])([O-])[O-] HCWCAKKEBCNQJP-UHFFFAOYSA-N 0.000 description 1
- 239000000395 magnesium oxide Substances 0.000 description 1
- 229910052919 magnesium silicate Inorganic materials 0.000 description 1
- 239000000391 magnesium silicate Substances 0.000 description 1
- 235000019792 magnesium silicate Nutrition 0.000 description 1
- 229910001092 metal group alloy Inorganic materials 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 229920000609 methyl cellulose Polymers 0.000 description 1
- 239000001923 methylcellulose Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 1
- 239000003921 oil Substances 0.000 description 1
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 1
- 150000002927 oxygen compounds Chemical class 0.000 description 1
- 229910003445 palladium oxide Inorganic materials 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 239000011574 phosphorus Substances 0.000 description 1
- 230000001376 precipitating effect Effects 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 229910052761 rare earth metal Inorganic materials 0.000 description 1
- 150000002910 rare earth metals Chemical class 0.000 description 1
- 239000011819 refractory material Substances 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 1
- 238000005549 size reduction Methods 0.000 description 1
- 238000007581 slurry coating method Methods 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 229910052642 spodumene Inorganic materials 0.000 description 1
- 230000006641 stabilisation Effects 0.000 description 1
- 238000011105 stabilization Methods 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 229910000314 transition metal oxide Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 description 1
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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/064—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof containing iron group metals, noble metals or copper
- B01J29/068—Noble metals
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
- B01D53/9404—Removing only nitrogen compounds
- B01D53/9409—Nitrogen oxides
- B01D53/9413—Processes characterised by a specific catalyst
- B01D53/9422—Processes characterised by a specific catalyst for removing nitrogen oxides by NOx storage or reduction by cyclic switching between lean and rich exhaust gases (LNT, NSC, NSR)
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
- B01D53/9445—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC]
- B01D53/945—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC] characterised by a specific catalyst
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
- B01D53/9459—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
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
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Abstract
公开了废气催化剂。一种废气催化剂包括贵金属和分子筛,并且具有下述红外光谱,该红外光谱除了该分子筛自身的吸收峰以外还具有750cm‑1至1050cm‑1的特征吸收峰。该废气催化剂也包括贵金属和分子筛,该贵金属量的大于5%位于该分子筛的孔隙内。该废气催化剂也包括第一和第二分子筛催化剂。该第一分子筛催化剂包括第一贵金属和第一分子筛,并且该第二分子筛催化剂包括第二贵金属和第二分子筛。该第一和第二分子筛不同。本发明也包括包含该废气催化剂的排气系统和利用该废气催化剂处理废气的方法。
Description
发明领域
本发明涉及废气吸附剂和其在用于内燃机的排气系统的用途。
发明背景
内燃机产生了包含各种污染物的废气,包括氮氧化物(“NOx”),一氧化碳和未燃烧的烃,这是政府立法的主题。排放控制系统广泛地用于降低排放到大气的这些污染物的量,一旦它们达到其操作温度(通常为200℃和更高),通常获得非常高的效率。然而,这些系统低于其操作温度(“冷启动”期间)是相对低效的。
例如,目前为了满足Euro 6b排放而实施的基于尿素的选择性催化还原(SCR)应用要求尿素定量给料位置处的温度大于约180℃,之后尿素可以定量给料和用于转化NOx。使用目前的系统难以解决低于180℃的NOx转化,并且未来欧洲和美国立法将强调低温NOx储存和转化。目前,这是通过加热策略来实现的,但是这具有有害的CO2排放的效应。
随着甚至更严格的国家和区域立法降低了可以从柴油或汽油发动机排放的污染物的量,在冷启动期间降低排放成为主要的挑战。因此,用于降低在冷启动条件过程中排放的NOx的水平的方法持续被探索。
例如,美国申请公开No.2012/0308439教导了一种冷启动催化剂,其包括:(1)沸石催化剂,其包含贱金属、贵金属、和沸石,和(2)负载的铂族金属催化剂,其包含一种或多种铂族金属和一种或多种无机氧化物载体。
PCT国际申请WO2008/047170公开了一种系统,其中来自贫燃废气的NOx在低于200℃的温度吸附和然后在高于200℃热脱附。教导NOx吸附剂由钯和铈氧化物或混合的氧化物或含铈和至少一种其它过渡金属的混合氧化物或复合氧化物组成。
美国申请公开No.2011/0005200教导一种催化剂系统,其通过将氨选择性催化还原(“NH3-SCR”)催化剂配制物置于贫燃NOx捕集器的下游来同时除去氨和加强净NOx转化率。教导NH3-SCR催化剂来吸附在贫燃NOx捕集器中富燃脉冲期间产生的氨。然后,储存的氨与从上游贫燃NOx捕集器排放的NOx反应,这提高了NOx转化率,同时消耗了储存的氨。
PCT国际申请WO2004/076829公开了废气纯化系统,其包括设置在SCR催化剂上游的NOx储存催化剂。NOx储存催化剂包含用至少一种铂族金属(Pt,Pd,Rh,或Ir)涂覆或活化的至少一种碱金属、碱土金属或稀土金属。教导特别优选的NOx储存催化剂包含用铂涂覆的氧化铈和此外在基于氧化铝的载体上的铂作为氧化催化剂。EP1027919公开了NOx吸附剂材料,其包含多孔载体材料,例如氧化铝,沸石,氧化锆,二氧化钛,和/或氧化镧,和至少0.1wt%的贵金属(Pt,Pd,和/或Rh)。例示了在氧化铝上负载的铂。
对于任何汽车系统和工艺,希望在废气处理系统中实现进一步的改善,特别是在冷启动的条件下。我们已经发现了能够在低温时段过程中减少冷启动排放的废气催化剂和系统。该新型废气催化剂也显示改善的耐硫性。
发明内容
本发明为废气催化剂,其对于在某个低温以下吸附NOx和烃(HC)并且在高于该低温的温度下转化并释放所吸附的NOx和HC有效。一种废气催化剂包括贵金属和分子筛,并且具有下述红外光谱,该红外光谱除了该分子筛自身的吸收峰以外还具有750cm-1至1050cm-1的范围内的特征吸收峰。该废气催化剂也包括贵金属和分子筛,该贵金属量的大于5%位于该分子筛的孔隙内。该废气催化剂也包括第一和第二分子筛催化剂。该第一分子筛催化剂包括第一贵金属和第一分子筛,并且该第二分子筛催化剂包括第二贵金属和第二分子筛,其中该第一和第二分子筛不同。本发明也包括包含该废气催化剂的排气系统和利用该废气催化剂处理废气的方法。
具体实施方式
本发明的废气催化剂对于在某个低温以下吸附NOx和烃(HC)并且在高于该低温的温度下转化并释放所吸附的NOx和HC有效。优选地,该低温在约200℃-250℃的范围内,更优选地约200℃。
本发明的一种废气催化剂包括贵金属和分子筛。该废气催化剂具有下述红外(IR)光谱,该红外光谱在750cm-1至1050cm-1的范围内、更优选地在800cm-1至1000cm-1的范围内、或者在850cm-1至975cm-1的范围内具有特征吸收峰。该特征吸收峰不包括该分子筛自身(即,未改性的分子筛)的IR光谱的吸收峰。
在另一实施方案中,本发明的废气催化剂包括贵金属和分子筛,其中该废气催化剂中的一些贵金属(添加的全部贵金属的大于1%)位于该分子筛的孔隙内。优选地,贵金属的总量的大于5%位于该分子筛的孔隙内;更优选地,可以是贵金属的总量的大于10%或大于25%或大于50%位于该分子筛的孔隙内。
另一实施方案中,本发明的废气催化剂包括贵金属和分子筛,并且具有下述的红外(IR)光谱,该红外光谱在750cm-1至1050cm-1的范围内(更优选地在800cm-1至1000cm-1的范围内、或者在850cm-1至975cm-1的范围内)具有特征吸收峰,并且该废气催化剂中的一些贵金属(添加的全部贵金属的大于1%、优选地添加的全部贵金属的大于5%)位于该分子筛的孔隙内。更优选地,该贵金属的总量的大于10%或大于25%或大于50%位于该分子筛的孔隙内。
该贵金属优选为钯、铂、铑、金、银、铱、钌、锇、或其混合物;更优选地,钯、铂、铑、或其混合物。特别优选钯。
该分子筛可以为任何天然或合成分子筛,包括沸石,和优选由铝、硅和/或磷组成。分子筛通常具有通过氧原子共享而连接的SiO4、AlO4和/或PO4的三维设置,但也可以为二维结构。分子筛骨架通常为阴离子型的,其通过电荷补偿阳离子来平衡,所述阳离子通常为碱和碱土元素(例如,Na,K,Mg,Ca,Sr,和Ba),铵离子以及质子。
优选地,该分子筛选自铝硅酸盐分子筛、金属置换的铝硅酸盐分子筛、铝磷酸盐分子筛、或金属置换的铝磷酸盐分子筛。
优选地,该分子筛为具有八个四面体原子的最大环尺寸的小孔隙分子筛、具有十个四面体原子的最大环尺寸的中孔隙分子筛、或具有十二个四面体原子的最大环尺寸的大孔隙分子筛。
如果该分子筛为小孔隙分子筛,则其优选为具有下述的骨架结构类型的分子筛:ACO、AEI、AEN、AFN、AFT、AFX、ANA、APC、APD、ATT、CDO、CHA、DDR、DFT、EAB、EDI、EPI、ERI、GIS、GOO、IHW、ITE、ITW、LEV、KFI、MER、MON、NSI、OWE、PAU、PHI、RHO、RTH、SAT、SAV、SIV、THO、TSC、UEI、UFI、VNI、YUG、和ZON、以及任何两种或更多种的混合物或共生物。更优选地,小孔隙沸石为AEI或CHA。特别优选的小孔隙分子筛的共生物包括KFI-SIV、ITE-RTH、AEW-UEI、AEI-CHA、和AEI-SAV。最优选地,小孔隙分子筛为AEI或CHA、或者AEI-CHA共生物。
如果该分子筛为中孔隙分子筛,其优选为具有MFI、FER、MWW、或EUO的骨架结构类型的分子筛。如果该分子筛为大孔隙分子筛,则其优选为具有CON、BEA、FAU、MOR、或EMT的骨架结构类型的分子筛。
可采用任何已知的方法制备废气催化剂。例如,贵金属可通过任何已知的方式添加至小孔分子筛以形成废气催化剂,添加的方式不认为是特别关键的。例如,贵金属化合物(例如硝酸钯)可通过浸渍、吸附、离子交换、初湿、沉淀等负载在分子筛上。其它金属也可以添加至废气催化剂。
优选地,该废气催化剂进一步包括流通式基材或过滤式基材。在一个实施方案中,该废气催化剂涂覆在流通式或过滤式基材上,和优选使用载体涂层程序沉积在流通式或过滤式基材上以产生该废气催化剂系统。
流通式或过滤式基材是能够包含催化组分的基材。基材优选为陶瓷基材或金属基材。陶瓷基材可由任何适合的耐火材料组成,例如,氧化铝,二氧化硅,二氧化钛,二氧化铈,氧化锆,氧化镁,沸石,氮化硅,碳化硅,锆硅酸盐,镁硅酸盐,铝硅酸盐,金属铝硅酸盐(例如堇青石和锂辉石),或其任何两种或更多种的混合物或混合的氧化物。堇青石、镁铝硅酸盐和碳化硅是特别优选的。
金属基材可由任何适合的金属组成,和特别是耐热的金属和金属合金例如钛和不锈钢以及含有铁、镍、铬和/或铝(除了其它痕量金属以外)的铁素体合金。
流通式基材优选为具有蜂窝状结构的流通式整料,所述蜂窝状结构具有多个小、平行的薄壁通道,其轴向穿过基材且从基材的入口或出口贯穿延伸。基材的通道横截面可为任何形状,但是优选正方形、正弦形、三角形、矩形、六边形、梯形、圆形或椭圆形。
过滤式基材优选为壁流式整料过滤器。壁流式过滤器的通道交替封闭,这允许废气物流从入口进入通道,然后流过通道壁,和从通向出口的不同通道离开过滤器。因此,废气物流中的颗粒被捕集在过滤器中。
废气催化剂可通过任何已知的方式添加至流通式或过滤式基材。使用载体涂层程序制备废气催化剂的代表性方法如下文所述。将理解的是,下文的方法可以根据不同的本发明实施方案而变化。
预成型的废气催化剂可通过载体涂覆步骤添加至流通式或过滤式基材。替代地,可通过将未改性分子筛首先载体涂覆在流通式或过滤式基材上以产生分子筛涂覆的基材来在所述基材上形成废气催化剂。然后,可以将贵金属添加至分子筛涂覆的基材,这可通过浸渍程序等完成。
优选通过首先在恰当的溶剂(优选水)中浆化细分的废气催化剂(或未改性小孔分子筛)颗粒以形成浆料来进行载体涂覆程序。额外组分例如过渡金属氧化物、粘合剂、稳定剂或助催化剂也可以作为水溶性或水分散性化合物的混合物引入浆料。浆料优选包含10-70重量%的固体,更优选20-50重量%。在形成浆料之前,废气催化剂(或未改性分子筛)颗粒优选经受尺寸减小处理(例如,研磨),使得固体颗粒的平均粒度为直径小于20微米。
然后,流通式或过滤式基材可一次或多次浸入浆料或浆料可涂覆在基材上,使得希望负载量的催化材料沉积在基材上。如果贵金属没有在载体涂覆流通式或过滤式基材之前引入分子筛,分子筛涂覆的基材通常干燥和煅烧,然后贵金属可通过任何已知的方式添加至分子筛涂覆的基材,包括浸渍、吸附或离子交换,例如,利用贵金属化合物(例如硝酸钯)。优选地,流通式或过滤式基材的整个长度用浆料涂覆,使得废气催化剂载体涂层覆盖基材整个表面。
在流通式或过滤式基材用废气催化剂涂覆和用贵金属浸渍(如果需要)之后,经涂覆的基材优选干燥和然后通过在升高的温度加热而煅烧以形成废气催化剂涂覆的基材。优选地,煅烧在400-600℃进行大约1-8小时。
在替代的实施方案中,流通式或过滤器基材包含废气催化剂。在这种情况下,废气催化剂挤出以形成流通式或过滤器基材。废气催化剂挤出的基材优选为蜂窝状流通式整料。
挤出的分子筛基材和蜂窝状体以及制备它们的方法在本领域中是已知的。参见例如,美国专利号5,492,883,5,565,394,和5,633,217和美国专利No.Re.34,804。通常,分子筛材料与持久粘合剂如有机硅树脂和临时粘合剂如甲基纤维素混合,和混合物挤出以形成蜂窝状生坯体,其然后煅烧和烧结以形成最终的分子筛流通式整料。分子筛可以在挤出之前包含贵金属,使得废气催化剂整料通过挤出程序而产生。替代地,贵金属可添加至预成型的分子筛整料以产生废气催化剂整料。
在另一实施方案中,该废气催化剂包括第一分子筛催化剂和第二分子筛催化剂。该第一分子筛催化剂包括第一贵金属和第一分子筛。该第二分子筛催化剂包括第二贵金属和第二分子筛。该第一和第二分子筛不同。本实施方案中,该废气催化剂可包括一种或多种的另外的分子筛催化剂(例如,第三分子筛催化剂和/或第四分子筛催化剂),条件是该另外的分子筛(一种或多种)不同于该第一和第二分子筛。
该第一贵金属和该第二贵金属独立地选自铂、钯、铑、金、银、铱、钌、锇、或其混合物;优选地,它们独立地选自钯、铂、铑、或其混合物。更优选地,该第一贵金属和该第二贵金属都为钯。
该第一分子筛优选为具有下述的骨架结构类型的小孔隙分子筛:ACO、AEI、AEN、AFN、AFT、AFX、ANA、APC、APD、ATT、CDO、CHA、DDR、DFT、EAB、EDI、EPI、ERI、GIS、GOO、IHW、ITE、ITW、LEV、KFI、MER、MON、NSI、OWE、PAU、PHI、RHO、RTH、SAT、SAV、SIV、THO、TSC、UEI、UFI、VNI、YUG、和ZON、以及任何两种或更多种的混合物或共生物。更优选地,小孔隙沸石为AEI或CHA。特别优选的小孔隙分子筛的共生物包括KFI-SIV、ITE-RTH、AEW-UEI、AEI-CHA、和AEI-SAV。最优选地,小孔隙分子筛为AEI或CHA、或者AEI-CHA共生物。
该第二分子筛优选为中或大孔隙分子筛。该中孔隙分子筛优选为具有MFI、FER、MWW、或EUO的骨架结构类型的分子筛。该大孔隙分子筛优选为具有CON、BEA、FAU、MOR、或EMT的骨架结构类型的分子筛。更优选地,该中或大孔隙分子筛为MFI或BEA。
可通过现有技术中公知的方法制备该废气催化剂。可将该第一分子筛催化剂和该第二分子筛催化剂物理地混合以制备该废气催化剂。优选地,该废气催化剂还包括流通式基材或过滤式基材。一个实施方案中,采用载体涂覆程序将该第一分子筛催化剂和该第二分子筛催化剂涂覆到该流通式或过滤式基材上,优选地沉积到该流通式或过滤式基材上以制备该废气催化剂系统。
适合的流通式或过滤式基材如上所述。
可通过任何已知的方法将该第一分子筛催化剂和该第二分子筛催化剂添加到该流通式或过滤式基材中。以下给出采用载体涂覆程序制备该废气催化剂的代表性方法。可理解下述的方法能够根据本发明的不同的实施方案而改变。而且,认为将该第一分子筛催化剂和该第二分子筛催化剂添加到该流通式或过滤式基材上的顺序并不关键。因此,可在该第二分子筛催化剂之前将该第一分子筛催化剂载体涂覆到该基材上或者可在该第一分子筛催化剂之前将该第二分子筛催化剂载体涂覆到该基材上或者将该第一分子筛催化剂和该第二分子筛催化剂同时载体涂覆到该基材上。
可通过载体涂覆步骤将该预成型的第一分子筛催化剂添加到该流通式或过滤式基材中。或者,可通过首先将未改性的分子筛载体涂覆到该基材上以制备分子筛涂覆的基材,从而在该流通式或过滤式基材上形成该第一分子筛催化剂。然后,可将贵金属添加到该分子筛涂覆的基材中,这可通过浸渍程序等而实现。
优选如上所述进行该载体涂覆程序。优选地,用该第一分子筛催化剂浆料涂覆该流通式或过滤式基材的整个长度以致该第一分子筛催化剂的载体涂层覆盖该基材的整个表面。
已用该第一分子筛催化剂浆料涂覆该流通式或过滤式基材,并且(如果需要)用贵金属浸渍后,优选将该涂覆的基材干燥,然后通过在升高的温度下加热从而煅烧以形成分子筛催化剂涂覆的基材。优选地,煅烧在400-600℃下进行约1-8小时。
该第二分子筛催化剂的载体涂层添加优选通过上述的程序实现。优选地,用负载PGM催化剂浆料涂覆该流通式或过滤式基材的整个长度以致该负载PGM催化剂的载体涂层覆盖该基材的整个表面。
已用该第一和第二分子筛催化剂浆料两者涂覆流通式或过滤式基材后,优选对其进行干燥,然后通过在升高的温度下加热而将其煅烧以制备该废气催化剂。优选地,煅烧在400-600℃下进行约1-8小时。
在备选的实施方案中,该流通式或过滤式基材包括该第一分子筛催化剂、该第二分子筛催化剂、或者该第一和第二分子筛催化剂两者。这种情况下,将该第一分子筛催化剂、第二分子筛催化剂、或者两种分子筛催化剂挤出以形成流通式或过滤式基材。如果没有包括在该挤出的基材中,则将该第一或第二分子筛催化剂涂覆到该挤出的流通式或过滤式基材上。该挤出的基材优选为蜂窝状流通式整块。
优选地,该废气催化剂包括包含该第一分子筛催化剂的第一层和包含该第二分子筛催化剂的第二层。典型地,可将该第一层设置在基材上并且将该第二层设置在该第一层上。或者,可将该第二层设置在基材上并且将该第一层设置在该第二层上。
在另一实施方案中,该废气催化剂包括包含该第一分子筛催化剂的第一区和包含该第二分子筛催化剂的第二区。该第一区可在该第二区的上游以致该第一区在该第二区之前接触该废气,或者该第二区可在该第一区的上游以致该第二区在该第一区之前接触该废气。优选地,该第二区位于该第一区的上游以致该废气在接触该第一分子筛催化剂之前接触该第二分子筛催化剂。这两个区可在相同的催化剂部件(或催化剂砖)上,或者包含该第一分子筛催化剂的第一区可位于与包含该第二分子筛催化剂的第二区的单独的砖(或催化剂组分)上。
本发明还包括用于包括废气催化剂的内燃机的排气系统。排气系统优选包括一个或多个另外的能够在正常操作温度从内燃机的废气除去污染物的后处理装置。优选地,排气系统包括废气催化剂和一种或多种选自以下的其它催化剂部件:(1)选择性催化还原(SCR)催化剂,(2)颗粒过滤器,(3)SCR过滤器,(4)NOx吸附催化剂,(5)三元催化剂,(6)氧化催化剂,或任何其组合。废气催化剂优选为独立于任何上述后处理装置的部件。替代地,废气催化剂可以作为部件引入任何上述后处理装置。
这些后处理装置在本领域是公知的。选择性催化还原(SCR)催化剂为通过与氮化合物(例如氨或尿素)或烃(贫燃NOx还原)反应将NOx还原为N2的催化剂。典型的SCR催化剂包含氧化钒-二氧化钛催化剂,氧化钒-钨氧化物-二氧化钛催化剂,或金属/沸石催化剂,例如铁/β沸石,铜/β沸石,铜/SSZ-13,铜/SAPO-34,Fe/ZSM-5,或铜/ZSM-5。
颗粒过滤器为减少来自内燃机的排气的颗粒的装置。颗粒过滤器包括催化颗粒过滤器和裸(非催化)颗粒过滤器。催化颗粒过滤器(用于柴油和汽油应用)包括金属和金属氧化物组分(例如Pt,Pd,Fe,Mn,Cu,和二氧化铈)以氧化烃和一氧化碳(除了破坏由过滤器捕集的烟灰之外)。
选择性催化还原过滤器(SCRF)是组合SCR和颗粒过滤器的功能的单一基材装置。它们用于降低来自内燃机的NOx和颗粒排放。除了SCR催化剂涂覆,颗粒过滤器也可以包括其它金属和金属氧化物组分(例如Pt,Pd,Fe,Mn,Cu和二氧化铈)以氧化烃和一氧化碳(除了破坏由过滤器捕集的烟灰之外)。
NOx吸附催化剂(NAC)设计以在贫燃排气条件下吸附NOx,在富燃条件下释放吸附的NOx,和还原释放的NOx以形成N2。NAC通常包括NOx-储存组分(例如,Ba,Ca,Sr,Mg,K,Na,Li,Cs,La,Y,Pr和Nd),氧化组分(优选Pt)和还原组分(优选Rh)。这些组分包含在一种或多种载体上。
三元催化剂(TWC)通常在化学计量条件下用于汽油发动机以在单一装置上将NOx转化为N2,将一氧化碳转化为CO2,以及将烃转化为CO2和H2O。
氧化催化剂和特别是柴油氧化催化剂(DOC)在本领域是公知的。氧化催化剂设计以将CO氧化为CO2以及将气相烃(HC)和柴油颗粒的有机馏分(可溶的有机馏分)氧化为CO2和H2O。典型的氧化催化剂包括在高表面积无机氧化物载体如氧化铝、二氧化硅-氧化铝和沸石上的铂以及任选的钯。
可以构造排气系统,使得废气催化剂设置成接近于发动机和额外的后处理装置设置在废气催化剂的下游。因此,在正常操作条件下,发动机废气首先流过废气催化剂,之后接触后处理装置。替代地,排气系统可以包含阀门或其它气体导向装置,使得在低温期间(通常低于约150-250℃,优选约200℃的温度,如在后处理装置处测量)引导废气接触后处理装置,之后流至废气催化剂。一旦后处理装置达到操作温度(约150-250℃,优选200℃,如在后处理装置处测量),然后再引导废气流接触废气催化剂,之后接触后处理装置。这确保废气催化剂的温度保持低,持续更长的时间,因此改善了废气催化剂的效率,同时允许后处理装置更快地达到操作温度。美国专利No.5,656,244例如教导了在冷启动和正常操作条件期间控制废气流的装置,该专利的教导通过参考引入本文。
本发明还包括一种处理来自内燃机的废气的方法。该方法包括在某个低温或低于该低温的温度将NOx和烃(HC)吸附在废气催化剂上,在高于所述低温的温度热脱附来自废气催化剂的NOx和HC,和在废气催化剂的下游的催化剂部件上催化除去脱附的NOx和HC。优选地,低温为约200℃-250℃,更优选约200℃。
废气催化剂的下游的催化剂部件为SCR催化剂、颗粒过滤器、SCR过滤器、NOx吸附催化剂、三元催化剂、氧化催化剂或其组合。
以下的实施例仅描述本发明。本领域技术人员将认识到在本发明精神和权利要求范围内的多个变型。
实施例1:贵金属分子筛催化剂的制备
根据下述通常的程序将钯添加到各种不同的分子筛中:通过使用硝酸钯作为前体对分子筛进行湿浸渍来制备粉末催化剂。在100℃下干燥后,将该样品在500℃下煅烧。然后在含有10%H2O的空气气氛中在750℃下将该样品水热老化。全部样品的Pd负载量为1wt.%。将分子筛负载Pd催化剂的实施例列于表1中。
实施例2:比较催化剂的制备
通过将Pd浸渍到CeO2载体上,并且在含有10%H2O的空气气氛中在750℃下水热老化,按照WO 2008/047170中报道的程序制备比较催化剂2A(Pd/CeO2)。Pd负载量为1wt.%。
实施例3:NOx储存能力测试程序
将该催化剂(0.4g)在以300L*hr-1*g-1的MHSV以2升/分流动的含有NO的气体混合物中在约80℃的吸附温度下保持2分钟。该吸附阶段后,在含有NO的气体的存在下以10℃/分钟的变温速率进行程序升温脱附(TPD)直至床温度达到约400℃以对所有储存的NOx的催化剂进行吹扫以进一步测试。然后从100℃的温度而不是80℃开始重复该试验;从150℃的温度开始再次重复该试验;并且从170℃的温度开始再次重复该试验。
在吸附和脱附两者的过程中含有NO的气体混合物包括12体积%O2、200ppm NO、5体积%CO2、200ppm CO、50ppm C10H22、和5体积%H2O。
将NOx储存计算为每升催化剂储存的NO2的量,针对于含有约3g/in3的催化剂负载量的整块。将不同温度下的结果示于表1中。
表1的结果表明所有分子筛负载催化剂,类似于比较催化剂2A,能够在低温下储存NOx。通常,小孔隙分子筛负载催化剂在高于150℃的温度下具有较高的NOx储存能力;而大孔隙分子筛负载催化剂在低于100℃的温度下具有较高的NOx储存能力。
实施例4:硫暴露测试程序后的NOx储存能力
通过在300℃下使废气催化剂1E、1H、和1K以及比较催化剂2A与含有SO2的气体(100ppm SO2、10%O2、5%CO2和H2O、余量N2)接触来对它们进行高水平的硫酸化以添加约64mg S每克催化剂。按照实施例3的程序,在100℃下测定硫酸化前后的催化剂的NOx储存能力。将结果列于表2中。
表2中所示的结果表明,本发明的废气催化剂即使在高水平的硫暴露后也保持显著量的NOx储存能力。相比之下,比较催化剂2A(Pd/CeO2)在相同的硫酸化条件下失去了其几乎全部NOx吸附能力。本发明的废气催化剂显示出显著改善的耐硫性。
实施例5:具有不同钯负载量的分子筛负载催化剂的制备和评价
按照实施例1的程序将钯添加到不同的分子筛中。使Pd负载量从0.25至2wt.%变动。在含有10%H2O的空气气氛中在750℃下对该样品进行水热老化。然后按照实施例3的程序对老化的样品测试它们的NOx储存能力。将在各个温度下的样品的NOx储存能力列于表3中。
表3中的结果表明增加的Pd负载量使NOx储存能力增大。
实施例6:混合分子筛负载钯催化剂的制备
首先按照实施例1的程序各自制备分子筛负载钯催化剂。随后以基于它们重量的当量比将这些催化剂彼此混合。然后在含有10%H2O的空气气氛中在750℃下将混合的催化剂水热老化。将混合的催化剂的实施例列于表4中。
实施例7:混合催化剂的评价
将个体催化剂(0.2g)和它们的混合物(0.4g)在以300L*hr-1*g-1的MHSV以2升/分流动的含有NO的气体混合物中在80℃的吸附温度下保持1分钟。该吸附阶段后,在含有NO的气体的存在下以100℃/分钟的变温速率进行程序升温脱附(TPD)直至床温度达到约400℃。吸附和脱附两者过程中含有NO的气体混合物包括12体积%O2、200ppm NO、5体积%CO2、200ppm CO、50ppm C10H22、和5体积%H2O。
在80℃下保持1分钟的过程中以及随后的从80至200℃的变温过程中计算NOx储存能力。将结果汇总于表4中。
表4中的结果表明通过将不同类型的分子筛负载贵金属催化剂组合,能够使不同温度下的NOx储存能力最优化。
实施例8:载体涂覆分子筛负载钯催化剂
按照实施例1的程序制备分子筛负载钯催化剂粉末。对于所有样品,Pd负载量为1.4wt.%。然后将每个粉末样品制成浆料并混合氧化铝粘结剂。将该混合物涂覆到流通式堇青石基材上以实现50g/ft3的Pd负载量。将涂覆的催化剂干燥,然后通过在500℃下加热4小时而将其煅烧。将催化剂的实施例列于表5中。
实施例9:与铂组分一起载体涂覆分子筛负载钯催化剂
进一步用氧化铝负载Pt催化剂的第二层涂覆实施例8中的载体涂覆的催化剂。将硝酸铂添加到氧化铝颗粒(研磨到直径小于10微米的平均粒径)的水浆中以形成Pt/氧化铝催化剂浆料。然后将该Pt/氧化铝催化剂浆料涂覆到Pd/分子筛涂覆的基材上以实现25g/ft3的Pt负载量,并且将最终的涂覆基材干燥,然后通过在500℃下加热4小时而将其煅烧。将含有Pt的催化剂的实施例也列于表5中。
实施例10:载体涂覆混合分子筛负载钯催化剂
按照实施例1的程序制备分子筛负载钯催化剂粉末。对于所有样品,Pd负载量为1.4wt.%。然后将两个选择的粉末样品制成浆料并以1:1的重量比混合,然后将氧化铝粘结剂添加到该混合的浆料中。将该混合物涂覆到流通式堇青石基材上以实现50g/ft3的Pd负载量。将涂覆的催化剂干燥,然后通过在500℃下加热4小时而将其煅烧。将催化剂的实施例列于表5中。
实施例11:与铂组分一起载体涂覆混合分子筛负载钯催化剂
进一步用氧化铝负载Pt催化剂的第二层涂覆实施例10中的载体涂覆的催化剂。将硝酸铂添加到氧化铝颗粒(研磨到直径小于10微米的平均粒径)的水浆中以形成Pt/氧化铝催化剂浆料。然后将该Pt/氧化铝催化剂浆料涂覆到Pd/分子筛涂覆的基材上以实现25g/ft3的Pt负载量,并且将最终的涂覆基材干燥,然后通过在500℃下加热4小时而将其煅烧。将含有Pt的催化剂的实例也列于表5中。
实施例12:载体涂覆的催化剂的评价
在流通式催化剂涂覆的堇青石基材的芯样品(直径2.54cm x长度7.62cm)上对所有载体涂覆的催化剂进行测试。首先在流通条件下在水热条件(5%H2O,余量空气)下750℃下的炉中将该催化剂芯老化16小时。然后使用通过调节各个废气组分的质量流量而制备的进料气体流,在实验室用反应器中对该芯测试催化活性。将该气体流量保持在21.2L min-1,产生30,000h-1的气时空速(GHSV=30,000h-1)。
使用由200ppm NO、200ppm CO、50ppm癸烷、10%O2、5%CO2、5%H2O和余量氮(体积%)组成的合成废气进料流,在贫燃条件下对该催化剂进行测试。将该催化剂暴露于该进料气体流,首先在80℃的等温入口气体温度下100秒,然后以100℃/min的变温速率将该入口气体温度升高到650℃。
将80℃下100秒期间和随后的从80至200℃的变温过程中的催化剂的NOx储存能力汇总于表5中。将低于200℃的温度下催化剂的累积HC储存和转化效率以及累积CO转化效率也汇总于表5中。
表5中的结果表明,大孔隙分子筛负载催化剂在低温下具有较高的NOx储存能力、而小孔隙分子筛负载催化剂在较高温度下具有较高的NOx储存能力。大孔隙分子筛负载催化剂也显示较高的HC储存和转化效率。将混合催化剂相对于具有对应的单一类型的分子筛组分的催化剂的结果进行比较,混合催化剂整体上在较宽的温度窗中保持高的NOx储存能力。
实施例13:分区催化剂的评价
通过将实施例9C中制备的Pd/BEA底部和Pt/Al2O3顶部催化剂的芯长度的一半与实施例9A中制备的Pd/CHA底部和Pt/Al2O3顶部催化剂的芯长度的一半组合来对分区的催化剂系统进行评价。实施例13A系统将实施例9C的芯的一半放置在实施例9A的芯的一半之前;而实施例13B系统将实施例9A的芯的一半放置在实施例9C的芯的一半之前。按照与实施例12中概述的程序相同的程序对这些系统进行评价。将评价结果汇总于表5中。
表5中的结果表明,分区的系统,特别是实施例11A,在比对应的个体催化剂宽得多的温度范围内显示高的NOx储存能力。
表1:NOx储存能力(g NO2/L)
*NM:未测定
**比较例
表2:NOx储存能力(g NO2/L)
*比较例
表3:NOx储存能力(g NO2/L)
*NM:未测定
表4:NOx储存能力(g NO2/L)
表5:载体涂覆催化剂的评价
Claims (13)
1.废气催化剂,其对于在某个低温以下吸附NOx和烃(HC)并且在高于该低温的温度下转化并释放所吸附的NOx和HC有效,所述废气催化剂包括第一分子筛催化剂和第二分子筛催化剂,其中该第一分子筛催化剂包括第一贵金属和第一分子筛,并且该第二分子筛催化剂包括第二贵金属和第二分子筛,其中该第一分子筛不同于该第二分子筛,其中该第一贵金属和该第二贵金属都为钯;和其中该第一贵金属的总量的大于5%位于该第一分子筛的孔隙内并且该第二贵金属的总量的大于5%位于该第二分子筛的孔隙内。
2.根据权利要求1所述的废气催化剂,其中该第一分子筛为选自以下骨架结构类型的小孔隙分子筛:ACO、AEI、AEN、AFN、AFT、AFX、ANA、APC、APD、ATT、CDO、CHA、DDR、DFT、EAB、EDI、EPI、ERI、GIS、GOO、IHW、ITE、ITW、LEV、KFI、MER、MON、NSI、OWE、PAU、PHI、RHO、RTH、SAT、SAV、SIV、THO、TSC、UEI、UFI、VNI、YUG和ZON、及两种或更多种的共生物。
3.根据权利要求2所述的废气催化剂,其中该小孔隙分子筛选自AEI和CHA的骨架结构类型。
4.根据权利要求1-3的任一项所述的废气催化剂,其中该第二分子筛为选自BEA和MFI的中或大孔隙分子筛。
5.根据权利要求1所述的废气催化剂,其中将该废气催化剂涂覆到流通式或过滤式基材上。
6.根据权利要求1所述的废气催化剂,其中将该废气催化剂挤出以形成流通式或过滤式基材。
7.根据权利要求1所述的废气催化剂,其中该废气催化剂包括包含该第一分子筛催化剂的第一层和包含该第二分子筛催化剂的第二层。
8.根据权利要求1所述的废气催化剂,其中该废气催化剂包括包含该第一分子筛催化剂的第一区和包含该第二分子筛催化剂的第二区。
9.根据权利要求8所述的废气催化剂,其中包含该第一分子筛催化剂的第一区位于与包含该第二分子筛催化剂的第二区分离的砖上。
10.内燃机用排气系统,其包括根据权利要求1-9的任一项所述的废气催化剂和催化剂组分,该催化剂组分选自:选择性催化还原(SCR)催化剂、颗粒过滤器、SCR过滤器、NOx吸附催化剂、三效催化剂、氧化催化剂、及其组合。
11.处理来自内燃机的废气的方法,所述方法包括在某个低温以下将NOx和烃(HC)吸附到根据权利要求1-9的任一项所述的废气催化剂上,在高于该低温的温度下将NOx和HC转化并且从该废气催化剂热脱附,和在该废气催化剂的下游的催化剂组分上将该脱附的NOx和HC催化去除。
12.根据权利要求11所述的方法,其中该低温在200℃-250℃的范围内。
13.根据权利要求11或权利要求12所述的方法,其中该第二分子筛催化剂位于该第一分子筛催化剂的上游以致该废气在接触该第一分子筛催化剂之前接触该第二分子筛催化剂。
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JP2015025433A (ja) † | 2013-07-29 | 2015-02-05 | 三菱自動車工業株式会社 | 内燃機関の排気浄化装置 |
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EP3077112B1 (en) | 2022-02-16 |
US10618003B2 (en) | 2020-04-14 |
WO2015085305A1 (en) | 2015-06-11 |
GB2522976A (en) | 2015-08-12 |
RU2680525C1 (ru) | 2019-02-22 |
KR102380570B1 (ko) | 2022-03-30 |
DE102014118096A1 (de) | 2015-06-11 |
GB2522976B (en) | 2017-03-01 |
KR20160094997A (ko) | 2016-08-10 |
GB201421740D0 (en) | 2015-01-21 |
CN105813745A (zh) | 2016-07-27 |
JP6438480B2 (ja) | 2018-12-12 |
EP3077112A1 (en) | 2016-10-12 |
BR112016012631B1 (pt) | 2021-05-04 |
JP2017505220A (ja) | 2017-02-16 |
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