CN103635249B - 用于内燃机的催化基体和排气*** - Google Patents
用于内燃机的催化基体和排气*** Download PDFInfo
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- CN103635249B CN103635249B CN201280030326.8A CN201280030326A CN103635249B CN 103635249 B CN103635249 B CN 103635249B CN 201280030326 A CN201280030326 A CN 201280030326A CN 103635249 B CN103635249 B CN 103635249B
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- oxide
- matrix
- zeolite
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- base metal
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- 238000002485 combustion reaction Methods 0.000 title claims abstract description 49
- 239000000758 substrate Substances 0.000 title abstract description 7
- 239000010457 zeolite Substances 0.000 claims abstract description 53
- 229910021536 Zeolite Inorganic materials 0.000 claims abstract description 50
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims abstract description 50
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims abstract description 46
- 239000010953 base metal Substances 0.000 claims abstract description 43
- 239000002184 metal Substances 0.000 claims abstract description 38
- 229910052751 metal Inorganic materials 0.000 claims abstract description 37
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims abstract description 34
- 239000010949 copper Substances 0.000 claims abstract description 28
- 229910052809 inorganic oxide Inorganic materials 0.000 claims abstract description 28
- 229910044991 metal oxide Inorganic materials 0.000 claims abstract description 17
- 229910052802 copper Inorganic materials 0.000 claims abstract description 16
- 150000004706 metal oxides Chemical class 0.000 claims abstract description 16
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims abstract description 15
- 238000000034 method Methods 0.000 claims abstract description 14
- 229910052742 iron Inorganic materials 0.000 claims abstract description 13
- 239000011159 matrix material Substances 0.000 claims description 132
- 238000006555 catalytic reaction Methods 0.000 claims description 55
- 239000007789 gas Substances 0.000 claims description 37
- 238000000605 extraction Methods 0.000 claims description 31
- 239000002912 waste gas Substances 0.000 claims description 30
- 239000000203 mixture Substances 0.000 claims description 23
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 15
- 230000003647 oxidation Effects 0.000 claims description 15
- 238000007254 oxidation reaction Methods 0.000 claims description 15
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 13
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical group O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims description 13
- 229910052697 platinum Inorganic materials 0.000 claims description 11
- 150000001875 compounds Chemical class 0.000 claims description 10
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 8
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 7
- 229910052763 palladium Inorganic materials 0.000 claims description 7
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 7
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 6
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 claims description 6
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 claims description 6
- 229910052703 rhodium Inorganic materials 0.000 claims description 6
- 239000010948 rhodium Substances 0.000 claims description 6
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims description 6
- 239000000377 silicon dioxide Substances 0.000 claims description 6
- 229910001928 zirconium oxide Inorganic materials 0.000 claims description 6
- 230000008859 change Effects 0.000 claims description 5
- 229910000476 molybdenum oxide Inorganic materials 0.000 claims description 5
- 229910000484 niobium oxide Inorganic materials 0.000 claims description 5
- URLJKFSTXLNXLG-UHFFFAOYSA-N niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Nb+5].[Nb+5] URLJKFSTXLNXLG-UHFFFAOYSA-N 0.000 claims description 5
- QGLKJKCYBOYXKC-UHFFFAOYSA-N nonaoxidotritungsten Chemical compound O=[W]1(=O)O[W](=O)(=O)O[W](=O)(=O)O1 QGLKJKCYBOYXKC-UHFFFAOYSA-N 0.000 claims description 5
- PQQKPALAQIIWST-UHFFFAOYSA-N oxomolybdenum Chemical compound [Mo]=O PQQKPALAQIIWST-UHFFFAOYSA-N 0.000 claims description 5
- 239000013618 particulate matter Substances 0.000 claims description 5
- 229910001930 tungsten oxide Inorganic materials 0.000 claims description 5
- 239000002131 composite material Substances 0.000 claims description 4
- 229910001657 ferrierite group Inorganic materials 0.000 claims description 4
- 229910052759 nickel Inorganic materials 0.000 claims description 4
- JYIBXUUINYLWLR-UHFFFAOYSA-N aluminum;calcium;potassium;silicon;sodium;trihydrate Chemical compound O.O.O.[Na].[Al].[Si].[K].[Ca] JYIBXUUINYLWLR-UHFFFAOYSA-N 0.000 claims description 3
- 238000009835 boiling Methods 0.000 claims description 3
- 229910001603 clinoptilolite Inorganic materials 0.000 claims description 3
- 229910052675 erionite Inorganic materials 0.000 claims description 3
- 239000012013 faujasite Substances 0.000 claims description 3
- 239000011572 manganese Substances 0.000 claims description 3
- 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 claims description 3
- 229910000480 nickel oxide Inorganic materials 0.000 claims description 3
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 claims description 3
- BPUBBGLMJRNUCC-UHFFFAOYSA-N oxygen(2-);tantalum(5+) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ta+5].[Ta+5] BPUBBGLMJRNUCC-UHFFFAOYSA-N 0.000 claims description 3
- 238000012545 processing Methods 0.000 claims description 3
- 239000004575 stone Substances 0.000 claims description 3
- PBCFLUZVCVVTBY-UHFFFAOYSA-N tantalum pentoxide Inorganic materials O=[Ta](=O)O[Ta](=O)=O PBCFLUZVCVVTBY-UHFFFAOYSA-N 0.000 claims description 3
- 229910052715 tantalum Inorganic materials 0.000 claims description 2
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims description 2
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims 1
- 150000002927 oxygen compounds Chemical class 0.000 claims 1
- 229910052726 zirconium Inorganic materials 0.000 claims 1
- 229930195733 hydrocarbon Natural products 0.000 abstract description 16
- 150000002430 hydrocarbons Chemical class 0.000 abstract description 16
- 239000004071 soot Substances 0.000 abstract description 8
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 abstract description 6
- 229910002091 carbon monoxide Inorganic materials 0.000 abstract description 6
- 238000010926 purge Methods 0.000 abstract description 3
- 230000001590 oxidative effect Effects 0.000 abstract description 2
- 239000003054 catalyst Substances 0.000 description 26
- 239000002002 slurry Substances 0.000 description 22
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 18
- 239000004215 Carbon black (E152) Substances 0.000 description 15
- 238000000576 coating method Methods 0.000 description 15
- 238000006243 chemical reaction Methods 0.000 description 14
- 238000003860 storage Methods 0.000 description 12
- 239000011248 coating agent Substances 0.000 description 11
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 11
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 8
- 238000010521 absorption reaction Methods 0.000 description 8
- 229910000037 hydrogen sulfide Inorganic materials 0.000 description 8
- 239000000463 material Substances 0.000 description 8
- 239000002245 particle Substances 0.000 description 8
- 239000003463 adsorbent Substances 0.000 description 7
- 229910021529 ammonia Inorganic materials 0.000 description 7
- 230000009467 reduction Effects 0.000 description 7
- 238000011144 upstream manufacturing Methods 0.000 description 7
- 238000006477 desulfuration reaction Methods 0.000 description 6
- 230000023556 desulfurization Effects 0.000 description 6
- 238000002360 preparation method Methods 0.000 description 6
- AKEJUJNQAAGONA-UHFFFAOYSA-N sulfur trioxide Chemical group O=S(=O)=O AKEJUJNQAAGONA-UHFFFAOYSA-N 0.000 description 6
- 229910001868 water Inorganic materials 0.000 description 6
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 5
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 description 5
- MCMNRKCIXSYSNV-UHFFFAOYSA-N ZrO2 Inorganic materials O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 5
- 239000012298 atmosphere Substances 0.000 description 5
- 238000001354 calcination Methods 0.000 description 5
- 235000019504 cigarettes Nutrition 0.000 description 5
- 238000007598 dipping method Methods 0.000 description 5
- 230000000694 effects Effects 0.000 description 5
- 238000005342 ion exchange Methods 0.000 description 5
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 5
- 230000008569 process Effects 0.000 description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 5
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 4
- -1 Sulphur compound Chemical class 0.000 description 4
- 230000032683 aging Effects 0.000 description 4
- 230000004323 axial length Effects 0.000 description 4
- 239000002585 base Substances 0.000 description 4
- 150000002739 metals Chemical class 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- 238000012360 testing method Methods 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 3
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 3
- 239000005864 Sulphur Substances 0.000 description 3
- 239000004411 aluminium Substances 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
- 229910052799 carbon Inorganic materials 0.000 description 3
- 229910002092 carbon dioxide Inorganic materials 0.000 description 3
- 239000012876 carrier material Substances 0.000 description 3
- 230000003197 catalytic effect Effects 0.000 description 3
- 239000003795 chemical substances by application Substances 0.000 description 3
- 229910052878 cordierite Inorganic materials 0.000 description 3
- 238000000151 deposition Methods 0.000 description 3
- 239000002283 diesel fuel Substances 0.000 description 3
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 description 3
- 238000001035 drying Methods 0.000 description 3
- 239000000446 fuel Substances 0.000 description 3
- 239000010410 layer Substances 0.000 description 3
- 238000001556 precipitation Methods 0.000 description 3
- 229910010271 silicon carbide Inorganic materials 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- 239000010936 titanium Substances 0.000 description 3
- 229910052719 titanium Inorganic materials 0.000 description 3
- 238000009736 wetting Methods 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 239000005749 Copper compound Substances 0.000 description 2
- 206010013786 Dry skin Diseases 0.000 description 2
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 2
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 2
- 229910002651 NO3 Inorganic materials 0.000 description 2
- GQPLMRYTRLFLPF-UHFFFAOYSA-N Nitrous Oxide Chemical compound [O-][N+]#N GQPLMRYTRLFLPF-UHFFFAOYSA-N 0.000 description 2
- 229910000831 Steel Inorganic materials 0.000 description 2
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 2
- 229910000323 aluminium silicate Inorganic materials 0.000 description 2
- 229940045985 antineoplastic platinum compound Drugs 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
- QVQLCTNNEUAWMS-UHFFFAOYSA-N barium oxide Inorganic materials [Ba]=O QVQLCTNNEUAWMS-UHFFFAOYSA-N 0.000 description 2
- TZCXTZWJZNENPQ-UHFFFAOYSA-L barium sulfate Chemical compound [Ba+2].[O-]S([O-])(=O)=O TZCXTZWJZNENPQ-UHFFFAOYSA-L 0.000 description 2
- 229910052791 calcium Inorganic materials 0.000 description 2
- 239000011575 calcium Substances 0.000 description 2
- 150000001768 cations Chemical class 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- 150000001880 copper compounds Chemical class 0.000 description 2
- 230000008021 deposition Effects 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 239000003502 gasoline Substances 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- PVFSDGKDKFSOTB-UHFFFAOYSA-K iron(3+);triacetate Chemical compound [Fe+3].CC([O-])=O.CC([O-])=O.CC([O-])=O PVFSDGKDKFSOTB-UHFFFAOYSA-K 0.000 description 2
- 229910052749 magnesium Inorganic materials 0.000 description 2
- 239000011777 magnesium Substances 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- RJIWZDNTCBHXAL-UHFFFAOYSA-N nitroxoline Chemical compound C1=CN=C2C(O)=CC=C([N+]([O-])=O)C2=C1 RJIWZDNTCBHXAL-UHFFFAOYSA-N 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 150000003058 platinum compounds Chemical class 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
- 231100000719 pollutant Toxicity 0.000 description 2
- 229910052700 potassium Inorganic materials 0.000 description 2
- 238000005245 sintering Methods 0.000 description 2
- 229910052708 sodium Inorganic materials 0.000 description 2
- 239000011734 sodium Substances 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 239000010959 steel Substances 0.000 description 2
- 229910052712 strontium Inorganic materials 0.000 description 2
- XTQHKBHJIVJGKJ-UHFFFAOYSA-N sulfur monoxide Chemical compound S=O XTQHKBHJIVJGKJ-UHFFFAOYSA-N 0.000 description 2
- 229910001017 Alperm Inorganic materials 0.000 description 1
- 241001466460 Alveolata Species 0.000 description 1
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- 229910052684 Cerium Inorganic materials 0.000 description 1
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 1
- 229910002588 FeOOH Inorganic materials 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 1
- 229910052779 Neodymium Inorganic materials 0.000 description 1
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 1
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 1
- 229910052777 Praseodymium Inorganic materials 0.000 description 1
- 229910018879 Pt—Pd Inorganic materials 0.000 description 1
- 229910052581 Si3N4 Inorganic materials 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 229910052783 alkali metal Inorganic materials 0.000 description 1
- 229910001413 alkali metal ion 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
- 229910001420 alkaline earth metal ion Inorganic materials 0.000 description 1
- 150000001342 alkaline earth metals Chemical class 0.000 description 1
- HZVVJJIYJKGMFL-UHFFFAOYSA-N almasilate Chemical compound O.[Mg+2].[Al+3].[Al+3].O[Si](O)=O.O[Si](O)=O HZVVJJIYJKGMFL-UHFFFAOYSA-N 0.000 description 1
- 229960003558 almasilate Drugs 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-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
- 150000001450 anions Chemical class 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 1
- CSSYLTMKCUORDA-UHFFFAOYSA-N barium(2+);oxygen(2-) Chemical compound [O-2].[Ba+2] CSSYLTMKCUORDA-UHFFFAOYSA-N 0.000 description 1
- 229910052792 caesium Inorganic materials 0.000 description 1
- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical compound [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 108020001778 catalytic domains Proteins 0.000 description 1
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- 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
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
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- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 238000003837 high-temperature calcination Methods 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 230000002779 inactivation Effects 0.000 description 1
- 229910001387 inorganic aluminate Inorganic materials 0.000 description 1
- 229910001959 inorganic nitrate Inorganic materials 0.000 description 1
- 150000002506 iron compounds Chemical class 0.000 description 1
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- 239000003949 liquefied natural gas Substances 0.000 description 1
- 239000003915 liquefied petroleum gas Substances 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
- 239000007769 metal material Substances 0.000 description 1
- 239000003863 metallic catalyst Substances 0.000 description 1
- 238000001465 metallisation Methods 0.000 description 1
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 239000002808 molecular sieve Substances 0.000 description 1
- QEFYFXOXNSNQGX-UHFFFAOYSA-N neodymium atom Chemical compound [Nd] QEFYFXOXNSNQGX-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000001272 nitrous oxide Substances 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 239000003921 oil Substances 0.000 description 1
- NDLPOXTZKUMGOV-UHFFFAOYSA-N oxo(oxoferriooxy)iron hydrate Chemical compound O.O=[Fe]O[Fe]=O NDLPOXTZKUMGOV-UHFFFAOYSA-N 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 238000010422 painting Methods 0.000 description 1
- GPNDARIEYHPYAY-UHFFFAOYSA-N palladium(ii) nitrate Chemical compound [Pd+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O GPNDARIEYHPYAY-UHFFFAOYSA-N 0.000 description 1
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 239000011574 phosphorus Substances 0.000 description 1
- 150000003057 platinum Chemical class 0.000 description 1
- 229920001296 polysiloxane Polymers 0.000 description 1
- 238000012805 post-processing Methods 0.000 description 1
- 239000011591 potassium Substances 0.000 description 1
- PUDIUYLPXJFUGB-UHFFFAOYSA-N praseodymium atom Chemical compound [Pr] PUDIUYLPXJFUGB-UHFFFAOYSA-N 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
- 238000010517 secondary reaction Methods 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon 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
- 239000002356 single layer Substances 0.000 description 1
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 1
- 239000002594 sorbent Substances 0.000 description 1
- 241000894007 species Species 0.000 description 1
- 229910052642 spodumene Inorganic materials 0.000 description 1
- 239000003381 stabilizer Substances 0.000 description 1
- 239000011232 storage material Substances 0.000 description 1
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 1
- 229910052815 sulfur oxide Inorganic materials 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
- 238000009941 weaving Methods 0.000 description 1
- 229910001845 yogo sapphire Inorganic materials 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
- 229910052649 zeolite group 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
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Abstract
公开了用于内燃机的排气***和用于排气***中的催化基体。该排气***包括贫燃NOx捕集器和催化基体。该催化基体具有第一区和第二区,其中该第一区包括负载在载体上的铂族金属,第二区包括负载在沸石上的铜或铁。第一区或第二区另外包括负载在无机氧化物上的贱金属氧化物或贱金属。还公开了使用该排气***处理来自内燃机的废气的方法。该排气***能够储存富燃吹扫(rich purging)中产生的NH3,使该NH3与从NOx捕集器滑过的NOx反应,控制NOx捕集器脱硫释放出的H2S,并氧化滑过的烃和一氧化碳。当该催化基体是过滤基体时,其还能够除去来自排气***的烟灰。
Description
发明领域
本发明涉及排气***及其在处理来自内燃机的排气中的应用,特别涉及可用于排气***中的催化基体组分。
发明背景
内燃机产生包含多种污染物(包括烃、一氧化碳、氮氧化物、硫氧化物和颗粒物质)的废气。越来越严格的国家和地区法律法规降低了能够从这种柴油或汽油发动机中排放出的污染物的量。已经由很多不同技术应用于排气***,在将废气排到大气中之前进行清洁。
典型的排气***包括:(1)NOx吸附催化剂(或“NOx捕集器”),用以吸附排气中的NOx;(2)氧化催化剂,用以氧化内燃机中未燃烧的烃和将CO转化为CO2;和(3)碳烟灰过滤器,用以在排放到大气中之前从废气中除去颗粒物。已经公开了这些***的各种组合。
美国申请公开号2011/0005200教导了一种催化剂***,其通过将氨选择性催化还原(“NH3-SCR”)催化剂配制物放置在贫燃NOx捕集器下游,在除去氨的同时提高了净NOx转化率。教导了NH3-SCR催化剂吸附在贫燃NOx捕集器中在富燃脉冲(rich pulse)过程中产生的氨。然后储存的氨与上游贫燃NOx捕集器排放出的NOx进行反应,这提高了NOx转化率,同时消耗了储存的氨。
美国申请公开号2011/0014099教导了可用于从主要在贫燃条件下操作的内燃机的废气中除去氮氧化物和颗粒物的颗粒物过滤器。该颗粒物过滤器包括过滤器体、铂族金属氧化催化剂活性涂层和位于第二涂层中的铜化合物。
PCT国际申请WO2008/075111教导了一种排气***,其包括(1)NOx吸附催化剂(“NAC”),(2)催化烟灰过滤器,(3)用于在正常贫燃运行操作过程中间歇性富集废气的装置,用以除去NAC上吸附的硫酸盐(作为H2S),和(4)位于至少一些NAC下游的化合物,其有效除去和/或转化富集的废气中至少一些产生的H2S。该H2S去除化合物可以位于排气***中的多个位置,包括:(a)NAC和催化烟灰过滤器之间,(b)NAC下游的基体,(c)催化烟灰过滤器上,(d)催化烟灰过滤器和排气***出口之间,和(e)(a)-(d)的各种组合。
PCT国际申请WO2010/114873公开了包含结合有选择性催化还原(“SCR”)催化剂的氨发生催化剂(例如NOx储存还原或贫燃NOx捕集器(“LNT”)催化剂)的排放处理***,及其与贫燃发动机一起使用的方法。LNT和SCR催化剂能够以各种构造使用。例如,LNT和SCR催化剂的位置能够为:(1)各自位于单独的基体块上,(2)位于单一基体块的前区和后区中,或者(3)位于SCR下游的柴油颗粒物过滤器上,使得各组分能够位于其各自的基体上,或者SCR能够涂覆在柴油颗粒物过滤器的前区或沿柴油颗粒物过滤器整个长度涂覆。
PCT国际申请WO2011/023332公开了废气后处理***,其具有壁流式过滤器作为组件(1)和其下游的流通式整料作为组件(2)。组件(1)和(2)具有至少一种对选自SOx、NOx、NH3、O2、烃和H2S的同一化合物的储存作用,其特征在于组件(2)中的储存容量设计使得在使用尽可能小的储存材料时,组件(2)下游的穿透信号具有满足考虑到废气化合物的各自的终端标准的浓度曲线的最高梯度。
对于任何汽车***和工艺,需要实现在废气处理***中更进一步的改进。我们发现了一种新的排气***和催化基体,其能够提供对来自内燃机的废气的增强的清洁。
发明概述
本发明是用于内燃机的排气***。该排气***包括贫燃NOx捕集器和催化基体。该催化基体具有第一区和第二区,其中该第一区包括负载在载体上的铂族金属,第二区包括负载在沸石上的铜或铁。第一区或第二区另外包括负载在无机氧化物上的贱金属氧化物或贱金属。本发明还包括催化基体本身。该催化基体是多功能组分,其储存富燃条件(吹扫)过程中在贫燃NOx捕集器中产生的NH3,使用该储存的NH3与滑过NOx捕集器的任何NOx反应,控制NOx捕集器脱硫释放出的H2S,并氧化滑过的烃和一氧化碳。在位于过滤器基体上时,该催化基体将实现从废气中除去烟灰的第六作用。
发明详述
本发明的排气***包括贫燃NOx捕集器和催化基体。贫燃NOx捕集器是现有技术中公知的(参见例如欧洲专利公开号0560991)。贫燃NOx捕集器是在贫燃排气条件下吸附NOx、在富燃条件下释放吸附的NOx并将释放的NOx还原生成N2的装置。
贫燃NOx捕集器典型地包括用于储存NOx的NOx吸附剂和氧化/还原催化剂。该氧化/还原催化剂通常包括一种或多种贵金属,优选铂、钯和/或铑。典型地,包括铂以实现氧化作用,包括铑以实现还原作用。
NOx储存组分优选包含碱土金属(例如钡、钙、锶和镁)、碱金属(例如钾、钠、锂和铯)、稀土金属(例如镧、钇、镨和钕)或其组合。这些金属典型地以氧化物形式存在。
该氧化/还原催化剂和NOx储存组分优选负载在排气***中所用的载体材料(例如无机氧化物)上。优选使用无机氧化物(例如氧化铝、氧化铈、氧化钛、氧化锆及其组合)作为该载体材料。
贫燃NOx捕集器实现三种功能。第一,在氧化催化剂存在下,一氧化氮与氧反应生成NO2。第二,NOx吸附剂将NO2以无机硝酸盐的形式吸附(例如,BaO或BaCO3在NOx吸附剂上转化为Ba(NO3)2)。最后,当发动机在富燃条件运行时,储存的无机硝酸盐分解生成NO或NO2,然后其通过与一氧化碳、氢和/或烃在还原催化剂存在下反应还原生成N2。典型地,在废气流中的热、一氧化碳和烃存在下氮氧化物转化为氮、二氧化碳和水。
在NOx捕集器中,NOx吸附剂和氧化/还原催化剂优选涂覆在流通式基体(优选蜂窝状整料)上。该流通式基体可以由陶瓷材料(例如堇青石)或金属材料制成。该贫燃NOx捕集器典型地设计以提供多个供汽车废气通过的通道。通道表面装填NOx吸附剂和氧化/还原催化剂。
NOx捕集器的组分可以通过任何已知方式添加。例如,载体材料、氧化-还原催化剂和NOx吸附剂材料优选可以施加并结合到基体上作为修补基面涂层(washcoat)、结合到基体表面上的多孔高表面积层。该修补基面涂层典型地是由水基浆料施加到基体上,然后干燥并高温煅烧。可选地,该修补基面涂层可以包含载体和NOx吸附剂,氧化-还原催化剂可以负载到经干燥的修补基面涂层载体层上(通过浸渍、离子交换等),然后进行干燥和煅烧。
尽管贫燃NOx捕集器在将来自内燃机的NOx转化为N2方面非常有效,但随着NOx吸附剂变得饱和,一些废气NOx将滑过该贫燃NOx捕集器。此外,在贫燃NOx捕集器中生成了一些副产物。例如,非选择性还原途径可能导致生成氨(NH3)和一氧化二氮(N2O),而不是所需的N2。这些不适宜的排放通常是需要避免或减少的。
次级反应还包括生成硫化氢。柴油或汽油染料中存在的硫化合物导致在废气中存在硫氧化物。在贫燃NOx捕集器中,在氧化催化剂上二氧化硫氧化为三氧化硫,NOx吸附剂与三氧化硫反应生成表面硫酸盐(例如,氧化钡或碳酸钡与三氧化硫反应生成硫酸钡)。这些硫酸盐比硝酸盐更稳定,且脱硫需要更高的温度,造成贫燃NOx捕集器的硫失活。脱硫能够通过各种技术实现,包括通过一系列短的富燃脉冲(“rich pulsing”)实现。在脱硫过程中,生成硫化氢和SO2。由于硫化氢不受欢迎的臭鸡蛋气味及其在较高浓度时的毒性,不希望其生成。因此,能使H2S以及NH3和N2O的含量最小化的任何排气***都是有利的。
除了贫燃NOx捕集器之外,本发明的排气***还包括具有第一区和第二区的催化基体。本发明还包括该催化基体本身。
该催化基体是包含催化剂组分的基体。该基体优选是陶瓷基体或金属基体。陶瓷基体可以由任何适合的耐火材料(例如氧化铝、二氧化硅、氧化钛、氧化铈、氧化锆、氧化镁、沸石、氮化硅、碳化硅、硅酸锆、硅酸镁、铝硅酸盐和金属铝硅酸盐(例如堇青石和锂辉石)或其任意两种或更多种的混合物或混合氧化物)制成。特别优选堇青石(铝硅酸镁)和碳化硅。
金属基体可以由任意适合的金属制成,特别是耐热金属和金属合金,例如钛和不锈钢以及包含铁、镍、铬和/或铝以及其他痕量金属的铁素体合金。
该基体优选是过滤器基体或流通式基体。特别地,该流通式基体是流通式整料,其优选具有蜂窝状结构,具有很多轴向通过基体延伸并延伸通过整个基体的小的平行的薄壁通道。该基体的通道横截面可以是任何形状,但优选是正方形、正弦曲线状、三角形、矩形、六角形、梯形、圆形或椭圆形。该基体最优选是流通式整料基体或过滤器基体。如果该基体是过滤器基体,其优选是壁流式整料过滤器。壁流式过滤器的通道交替阻断,这样使废气流从入口进入通道,然后流过通道壁,从通向出口的不同通道离开过滤器。由此将废气流中的颗粒物捕集在过滤器中。
该基体包含两个催化区,各区包含沉积在基体上的不同的催化剂组合物。优选地,基体上的这两个区很少重叠或者没有重叠。例如,第一区可以覆盖基体总长度的10-90%,第二区将会覆盖该基体的剩余长度(即未被第一区覆盖的剩余的90-10%)。更优选地,第一区覆盖基体总长度的40-60%,第二区覆盖该基体的剩余长度(即未被第一区覆盖的剩余的60-40%)。在使用壁流式整料过滤器时,一个区可以位于入口通道中,另一个区可以位于出口通道中,由此有效分隔开第一区和第二区。区的涂覆方法公开于例如PCT国际申请WO99/47260。
第一区包括负载在载体上的铂族金属。铂族金属优选是铂、钯、铑或其混合物;最优选地,铂族金属是铂、钯及其混合物。该载体优选是沸石、无机氧化物或其混合物。更优选地,该载体是无机氧化物,例如氧化铝、二氧化硅、氧化钛、氧化锆、氧化铈、氧化铌、钽氧化物、钼氧化物、钨氧化物、其任意两种或更多种的混合氧化物或复合氧化物(例如二氧化硅-氧化铝、氧化铈-氧化锆或氧化铝-氧化铈-氧化锆)及其混合物。特别优选氧化铈-氧化锆混合氧化物。
第二区包括负载在沸石上的铜或铁,包括铜和铁的混合物。该沸石可以是任何天然或合成沸石,包括分子筛,优选由铝、硅和/或磷构成。该沸石典型地具有通过共享氧原子而连接的SiO4、AlO4和/或PO4的三维排列。该沸石框架典型地是阴离子的,其通过电荷互补的阳离子进行平衡,阳离子典型地为碱金属和碱土金属元素(例如Na、K、Mg、Ca、Sr和Ba)以及质子。也可以将其他金属(例如Fe、Ti和Ga)引入沸石骨架中制备引入金属的沸石(例如钛硅沸石(titanosilicalite))。第二区优选可以包括一种或多种铂族金属,优选铂、钯或铑,但如果使用,铂族金属在第二区中的总负载量将较低,小于1g/ft3(0.035g/L)。
沸石优选是β沸石、八面沸石(例如X-沸石或Y-沸石,包括NaY和USY)、L-沸石、ZSM沸石(例如ZSM-5、ZSM-48)、SSZ-沸石(例如SSZ-13、SSZ-41、SSZ-33)、镁碱沸石、丝光沸石、菱沸石、硅铝钾沸石、毛沸石、斜发沸石、硅质岩、磷酸铝沸石(包括金属铝磷酸盐,例如SAPO-34)、中孔沸石(例如MCM-41、MCM-49、SBA-15)或其混合物;更优选地,该沸石是β沸石、镁碱沸石或菱沸石。
第一区或第二区另外包括负载在无机氧化物上的贱金属氧化物或贱金属。贱金属优选是铁、锰、铜、镍或其混合物。无机氧化物优选是氧化铝、二氧化硅、氧化钛、氧化锆、氧化铈、氧化铌、钽氧化物、钼氧化物、钨氧化物、其任意的混合氧化物或复合氧化物及其混合物。特别优选氧化铝。该贱金属氧化物优选是铁氧化物、锰氧化物、铜氧化物、镍氧化物或其混合物,由此能够将贱金属氧化物(例如铁氧化物)的颗粒单独添加到第一区或第二区中。
优选地,该贱金属位于第二区上,使得该第二区包括位于沸石上的铜或铁和位于无机氧化物上的贱金属氧化物或贱金属。当贱金属位于第一区中时,最优选该贱金属与铂族金属物理分隔开。因此,将负载的铂族金属和负载在无机氧化物上的贱金属氧化物或贱金属的颗粒分开添加到第一区,以将第一区中的这两种催化剂物理分隔开。
本发明的催化基体可以通过现有技术中公知的工艺制备。优选地,使用修补基面涂覆工艺将催化区置于基体上。下面提出了使用修补基面涂覆工艺制备催化基体的代表性工艺。应当理解,下面的工艺能够依照本发明的不同实施方案变化。而且,第一区和第二区添加到基体上的顺序并不重要。因此,可以在修补基面涂覆第二区之前将第一区修补基面涂覆在基体上,或者可以在修补基面涂覆第一区之前将第二区修补基面涂覆在基体上。
催化基体的第一区优选使用修补基面涂覆工艺制备。在修补基面涂覆步骤之前可以将铂族金属添加到载体上,或者可以在将载体修补基面涂覆到基体上之后将铂族金属添加到涂覆有载体的基体上。如果在修补基面涂覆该基体的第一区之前将铂族金属添加到载体上,则能够通过任何已知的方式将其负载到载体上,添加方式并不是特别关键。例如,可以通过浸渍、吸附、离子交换、初始润湿、沉淀等将铂化合物(例如硝酸铂)负载在载体上。
修补基面涂覆优选通过首先将负载的铂族金属(或仅载体)的磨碎颗粒在适合的溶剂(优选水)中浆料化以生成浆料而实现。该浆料优选包含5-70wt%固体,更优选10-50wt%。优选地,在形成浆料之前,将载体或铂族金属/载体颗粒磨碎或经过另一粉碎工艺以确保基本上全部固体颗粒具有平均直径小于20微米的粒度。也可以将其他组分(例如稳定剂或促进剂)作为水溶性或水分散性化合物或络合物的混合物加入浆料中。
然后可以用该浆料将该基体涂覆一次或多次,使得在该基体上将沉积所需负载量的催化材料。如果仅将载体沉积在基体上,则然后可以通过任何已知方式将铂族金属添加到涂覆有载体的基体上,包括铂化合物(例如硝酸铂)的浸渍、吸附或离子交换。优选地,用该浆料涂覆该基体,使得第一区仅占基体轴向长度的10-90%,更优选地占基体轴向长度的40-60%。
在用该浆料涂覆基体的第一区并如果需要的话用铂族金属浸渍之后,典型地通过在优选80-150℃的升高温度加热来干燥经涂覆的基体。也可以在更高的温度(例如400-600℃)煅烧该基体,但在添加第二区之前通常并不需要煅烧。
如果将贱金属添加到第一区中,则优选将负载的铂族金属和贱金属氧化物(或贱金属/无机氧化物)负载到基体上,使这两种催化剂在第一区内物理分隔开。这可以通过任何已知的方式实现,但优选将贱金属氧化物(或贱金属/无机氧化物)作为与铂族金属的添加分开的修补基面涂覆步骤添加到第一区中。如果使用贱金属/无机氧化物,优选在修补基面涂覆第一区之前将该贱金属负载到无机氧化物上(例如,通过浸渍、吸附、离子交换、初始润湿、沉淀等将贱金属化合物(例如乙酸铁)负载在无机氧化物上)。可选地,可以通过修补基面涂覆包含贱金属氧化物(或贱金属/无机氧化物)和负载的铂族金属的不同颗粒的浆料同时添加铂族金属和贱金属。
如果将贱金属添加到第一区中,则通过在优选80-150℃的升高温度加热来干燥基体。也可以在更高温度(例如400-600℃)煅烧基体,但通常并不需要煅烧。
优选使用修补基面涂覆工艺制备催化基体的第二区。优选在修补基面涂覆基体的第二区之前,通过任何已知方式将铜或铁负载到沸石上以形成Cu(Fe)/沸石物类,添加方式并是特别关键。例如,可以通过浸渍、吸附、离子交换、初始润湿、沉淀等将铜化合物(例如乙酸铜)或铁化合物(例如乙酸铁)负载在该沸石上。也可以将其他金属添加到该Cu(Fe)/沸石组合上。
优选将贱金属氧化物(或贱金属/无机氧化物)添加到第二区。优选地,将Cu(Fe)/沸石和贱金属氧化物(或贱金属/无机氧化物)的磨碎颗粒在适当的溶剂(优选水)中浆料化。优选地,在形成浆料之前,将Cu(Fe)/沸石和贱金属氧化物(或贱金属/无机氧化物)的颗粒磨碎或经过另一粉碎工艺以确保基本上全部固体颗粒具有平均直径小于20微米的粒度。也可以将其他组分(例如稳定剂或促进剂)作为水溶性或水分散性化合物或络合物的混合物加入浆料中。
然后可以用Cu(Fe)/沸石和贱金属的浆料将该基体(在基体沉积第一区的相反端)涂覆一次或多次,使得在该基体上将沉积所需负载量的催化材料。可选地,可以将Cu(Fe)/沸石和贱金属物类作为单独的层添加在基体上。例如,可以首先在基体上沉积仅包含铜Cu(Fe)/沸石的浆料的基层,然后涂覆贱金属物类的顶层,或者相反的层叠方案。
优选地,用第二区浆料涂覆该基体使得该第二区和第一区很少重叠或没有重叠。第二区优选将仅占基体轴向长度的10-90%,更优选占基体轴向长度的40-60%。
在用第二浆料涂覆过该基体之后,典型地通过在升高温度加热来干燥并然后煅烧。优选地,煅烧在400-600℃发生约1-8小时。
在某些情况中,优选可以在基体上添加小的第三区,使得该第三区(优选占基体轴向长度的少于20%,更优选少于10%)位于第二区之后并位于基体上与第三区相对的端。当该基体是过滤器基体且第一区位于排气***中在第二区之前接触排气使得烟灰在高温燃烧过程中生成的烃和CO在第二区上不能完全燃烧时,第三区可能是特别有用的。如果使用,第三区将包含铂族金属,优选铂、钯和/或铑,以有助于任何烃和CO的氧化。
催化基体优选位于排气***中使其位于贫燃NOx捕集器的下游,使得废气在接触催化基体之前接触贫燃NOx捕集器。优选地,该双区催化基***于排气***中使得废气在离开贫燃NOx捕集器之后与上游(入口)区接触,且在上游区之后存在下游(出口)区。接触来自贫燃NOx捕集器的废气的上游区可以是催化基体的第一区或第二区。因此,第一区能够经取向以在第二区之前接收来自NOx捕集器的废气;或者第二区能够经取向以在第一区之前接收来自NOx捕集器的废气。优选地,该催化基体的第一区经取向以在第二区之前接收来自NOx捕集器的废气,使得离开贫燃NOx捕集器的废气在接触负载在沸石上的铜或铁之前接触铂族金属催化剂。
该双区催化基体在排气***中实现五个不同的作用。第一,用该铜沸石组分储存在富燃条件(吹扫)过程中在贫燃NOx捕集器中生成的NH3。第二,储存的NH3将与通过NOx捕集器的任何滑过的NOx反应。因此,不仅减少了排放到大气中的氨量,而且通过本发明的排气***还优化了该排气***的NOx转化率。第三,该催化基体通过将其氧化为SO2控制了NOx捕集器脱硫释放的H2S。第四,铂族金属催化剂氧化在接触催化基体之前未转化的烃(“滑过的烃”)。第五,铂族金属催化剂氧化在催化基体之前未转化的滑过的一氧化碳。
优选地,该催化基体是过滤器基体。当其是过滤器基体时,该催化基体实现了从废气中除去烟灰的第六个作用。
如果该催化基体是流通式基体,则本发明的排气***优选包括颗粒物过滤器,更优选催化烟灰过滤器。当存在时,该颗粒物过滤器优选能够收集烟灰,而不会在排气***中造成过高的背压。通常,能够使用陶瓷、烧结金属或织造或非织造的金属丝过滤器,特别优选壁流式蜂窝状结构。该过滤器的结构材料优选是多孔陶瓷、碳化硅或烧结金属。该过滤器能够具有催化功能,例如其可以包括氧化铝涂层和/或贱金属催化剂,例如La/Cs/V2O5。烟灰通常是含碳的可溶有机馏分和/或挥发性有机馏分和/或重烃。烟灰燃烧生成CO2和H2O。
如果使用,该颗粒物过滤器可以位于催化基体的上游或下游。优选地,该颗粒物过滤器位于催化基体的上游和贫燃NOx捕集器的下游,使得来自内燃机的废气通过贫燃NOx捕集器,然后通过颗粒物过滤器,然后在排出到大气之前通过催化基体。
本发明还包括处理来自内燃机的废气,特别用于处理来自车辆贫燃内燃机(例如柴油发动机、贫燃汽油发动机或者液态石油气或天然气驱动的发动机)的废气。该方法包括使废气流过贫燃NOx捕集器和该催化基体。
以下实施例仅作为本发明的示例。本领域技术人员将认识到,在本发明的精神和权利要求的范围内存在许多变型。
实施例1:制备催化基体
如下制备具有区1和区2的催化基体:
区1(CeO2-ZrO2+Al2O3+沸石上的Pt-Pd):将氧化铝(粒度d90小于10微米)的含水浆料与铂盐和硝酸钯的水溶液合并。然后在该浆料中添加氧化铈-氧化锆混合氧化物(粒度d90小于10微米),然后添加β沸石以得到氧化铝:混合氧化物:沸石为4:3:3的最终组成。将该浆料修补基面涂覆到3.0L体积的钛酸铝壁流式过滤器(300单元/平方英寸(46.5单元cm-2))的入口通道上,并在空气中在100℃干燥。区1中的最终总涂覆负载量为0.55g/in3(33.6g/L),铂族金属负载量为45g/ft3(1.59g/L;Pt:Pd质量比=2:1)。
区2(Cu/沸石和氧化铁):将氧化铝(粒度d90小于10微米)的含水浆料与Cu交换沸石和氧化铁颗粒(FeOOH,d90小于10微米)的浆料合并,得到氧化铝:沸石:氧化铁为4:3:3的最终组成。将该浆料涂覆到该壁流式过滤器的出口通道上,在空气中在100℃干燥,然后在500℃煅烧。区2中的最终涂覆负载量为0.5g/in3(30.5g/L),铜负载量为12g/ft3(0.42g/L),铁负载量为250g/ft3(8.83g/L)。
实施例2:测试程序
使用标准程序将发动机老化的(engine-aged)贫燃NOx捕集器(LNT)和实施例1的催化基体安装在不锈钢罐中并出于紧连接位置,并且安装到台式安装的2.0升普通轨式柴油发动机的排气***上。在安装到测试设备中之前将该发动机老化的LNT在800℃在空气中进行热炉老化,在使用之前将该催化基体在800℃在空气中进行水热炉老化(在水存在下)。该催化基***于该***中LNT的下游,其取向使得来自LNT的废气在接触区2之前首先接触区1(在下表中列为基体1A)。将该发动机以常规方式连接到功率计上,发动机和功率计都由计算机控制。以1秒间隔测定LNT上游、LNT之后和催化基体之后的废气排放量。
NOx、CO和烃转化率和最高NH3测量值:使该发动机运行经过三次MVEG-B驱动循环,测定全部三次MVEG循环中最高NH3值和NOx、CO和烃(HC-非甲烷的烃)排放的转化率,以在稳定条件下测试。结果示于表1(最高NH3)和表2(NOx、CO和HC转化率)中。
最高H2S测试:在稳态仅贫燃条件下使该发动机以2000rpm和70Nm扭矩运行,使用包含350ppm S的柴油燃料,得到300℃的NOx捕集器入口温度。该仅贫燃条件在NOx捕集器上生成硫酸盐,捕集器中的目标硫负载量为1g S。在仅贫燃条件下,将NOx捕集器入口温度提高到550℃,然后在2000rpm和70Nm进行脱硫,使用贫燃/富燃快速变换(摆动)10分钟,得到700-750℃的床温。测定LNT之后和催化基体之后的H2S。
在组合***上重复上述测试条件,其中该催化基***于***中使得来自LNT的废气在接触区1之前首先接触区2(在下表中列为基体1B)。
结果(参见表1)显示,催化基体(1A和1B)显著降低了废气流中的NH3量,还显著降低了测定的来自脱硫的H2S量,特别是对于使区1首先接触的基体1A来说。结果还显示,在将催化基体(1A和1B)放在LNT之后时,还提高了NOx、HC和CO的转化率。例如结果显示,基体1A和1B在LNT之后进一步将HC转化率另外提高了11%,由此有效地将总HC转化率从在LNT上转化的59%提高至70%。
表1:氨气和硫化氢结果
表2:经过MVEG循环的NOx、烃和CO转化率
Claims (16)
1.用于内燃机的排气***,包括:
(a)贫燃NOx捕集器;和
(b)具有第一区和第二区的催化基体,其中该第一区包括负载在载体上的铂族金属,第二区包括负载在沸石上的铜或铁,第二区另外包括负载在无机氧化物上的贱金属氧化物或贱金属,其中所述无机氧化物为氧化铝、二氧化硅、氧化钛、氧化锆、氧化铈、氧化铌、钽氧化物、钼氧化物、钨氧化物、其任意的混合氧化物或复合氧化物及其混合物,并且,其中将该催化基体取向为使得来自NOx捕集器的废气在接触第二区之前接触第一区。
2.权利要求1的排气***,其中该基体是过滤器基体。
3.权利要求1的排气***,其中该基体是流通式基体,且该排气***进一步包括颗粒物过滤器。
4.权利要求1的排气***,其中该沸石选自β沸石、八面沸石、L-沸石、ZSM沸石、SSZ-沸石、镁碱沸石、丝光沸石、菱沸石、硅铝钾沸石、毛沸石、斜发沸石、硅质岩、磷酸铝沸石、中孔沸石及其混合物。
5.权利要求1-4中任一项的排气***,其中该铂族金属选自铂、钯、铑及其混合物,且该载体为无机氧化物。
6.权利要求5的排气***,其中所述无机氧化物为氧化铝、二氧化硅、氧化钛、氧化锆、氧化铈、氧化铌、钽氧化物、钼氧化物、钨氧化物、其任意两种或更多种的混合氧化物或复合氧化物及其混合物。
7.权利要求5的排气***,其中所述无机氧化物为沸石。
8.权利要求5的排气***,其中该贱金属选自铁、锰、铜、镍及其混合物,且该贱金属氧化物选自铁氧化物、锰氧化物、铜氧化物、镍氧化物及其混合物。
9.具有第一区和第二区的催化基体,其中该第一区包括负载在载体上的铂族金属,第二区包括负载在沸石上的铜或铁,第二区另外包括负载在无机氧化物上的贱金属氧化物或贱金属,其中将该催化基体取向为使得来自NOx捕集器的废气在接触第二区之前接触第一区。
10.权利要求9的催化基体,其中该基体是过滤器基体或流通式基体。
11.权利要求9的催化基体,其中该沸石选自β沸石、八面沸石、L-沸石、ZSM沸石、SSZ-沸石、镁碱沸石、丝光沸石、菱沸石、硅铝钾沸石、毛沸石、斜发沸石、硅质岩、磷酸铝沸石、中孔沸石及其混合物。
12.权利要求9-11中任一项的催化基体,其中该铂族金属选自铂、钯及其混合物,且该载体为无机氧化物。
13.权利要求11的催化基体,其中所述无机氧化物为氧化铝、二氧化硅、氧化钛、氧化锆、氧化铈、氧化铌、钽氧化物、钼氧化物、钨氧化物、其任意两种或更多种的混合氧化物或复合氧化物及其混合物。
14.权利要求11的催化基体,其中所述无机氧化物为沸石。
15.权利要求9-11中任一项的催化基体,其中该贱金属选自铁、锰、铜、镍及其混合物,且该贱金属氧化物选自由铁氧化物、锰氧化物、铜氧化物、镍氧化物及其混合物。
16.处理来自内燃机的废气的方法,包括使该废气流过贫燃NOx捕集器和权利要求9的催化基体。
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KR20140048163A (ko) | 2014-04-23 |
GB2504897A (en) | 2014-02-12 |
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US8795617B2 (en) | 2014-08-05 |
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WO2012175948A1 (en) | 2012-12-27 |
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EP2723476B1 (en) | 2020-07-29 |
GB2492175B (en) | 2018-06-27 |
BR112013032528A2 (pt) | 2017-07-04 |
JP2014525822A (ja) | 2014-10-02 |
US20140044630A1 (en) | 2014-02-13 |
US8540952B2 (en) | 2013-09-24 |
DE112012002601T5 (de) | 2014-03-20 |
RU2609796C2 (ru) | 2017-02-06 |
KR20190052715A (ko) | 2019-05-16 |
JP6134708B2 (ja) | 2017-05-24 |
GB201320549D0 (en) | 2014-01-08 |
KR102010602B1 (ko) | 2019-08-13 |
CN103635249A (zh) | 2014-03-12 |
US20130149220A1 (en) | 2013-06-13 |
GB201111950D0 (en) | 2011-08-24 |
KR102076996B1 (ko) | 2020-02-13 |
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