WO2023198570A1 - Système de gaz d'échappement pour moteurs à allumage par étincelle fonctionnant principalement de manière stœchiométrique, comprenant un catalyseur permettant de réduire les émissions d'ammoniac - Google Patents
Système de gaz d'échappement pour moteurs à allumage par étincelle fonctionnant principalement de manière stœchiométrique, comprenant un catalyseur permettant de réduire les émissions d'ammoniac Download PDFInfo
- Publication number
- WO2023198570A1 WO2023198570A1 PCT/EP2023/059079 EP2023059079W WO2023198570A1 WO 2023198570 A1 WO2023198570 A1 WO 2023198570A1 EP 2023059079 W EP2023059079 W EP 2023059079W WO 2023198570 A1 WO2023198570 A1 WO 2023198570A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- exhaust system
- osc
- ammonia
- exhaust gas
- metal catalyst
- Prior art date
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- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 title claims abstract description 190
- 229910021529 ammonia Inorganic materials 0.000 title claims abstract description 92
- 239000003054 catalyst Substances 0.000 title claims description 88
- 238000002485 combustion reaction Methods 0.000 title claims description 20
- 239000007789 gas Substances 0.000 claims description 54
- 239000010457 zeolite Substances 0.000 claims description 44
- 230000003197 catalytic effect Effects 0.000 claims description 43
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 41
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 39
- 229910000510 noble metal Inorganic materials 0.000 claims description 27
- 229910052760 oxygen Inorganic materials 0.000 claims description 26
- 239000001301 oxygen Substances 0.000 claims description 26
- 239000010970 precious metal Substances 0.000 claims description 26
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 25
- 239000000463 material Substances 0.000 claims description 19
- 229910052763 palladium Inorganic materials 0.000 claims description 19
- 229910052697 platinum Inorganic materials 0.000 claims description 19
- 239000010948 rhodium Substances 0.000 claims description 18
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 16
- 229910052703 rhodium Inorganic materials 0.000 claims description 15
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims description 15
- 239000011232 storage material Substances 0.000 claims description 13
- 229910052742 iron Inorganic materials 0.000 claims description 8
- 238000000034 method Methods 0.000 claims description 7
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 6
- 229910052802 copper Inorganic materials 0.000 claims description 6
- 239000010949 copper Substances 0.000 claims description 6
- 229910001428 transition metal ion Inorganic materials 0.000 claims description 2
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 28
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 26
- 238000000576 coating method Methods 0.000 description 23
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 22
- 238000003860 storage Methods 0.000 description 22
- 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 21
- 229910052684 Cerium Inorganic materials 0.000 description 20
- 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 20
- 239000010410 layer Substances 0.000 description 20
- QVQLCTNNEUAWMS-UHFFFAOYSA-N barium oxide Chemical compound [Ba]=O QVQLCTNNEUAWMS-UHFFFAOYSA-N 0.000 description 18
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 17
- 229910052761 rare earth metal Inorganic materials 0.000 description 17
- 150000002910 rare earth metals Chemical class 0.000 description 17
- 229910052726 zirconium Inorganic materials 0.000 description 17
- GQPLMRYTRLFLPF-UHFFFAOYSA-N Nitrous Oxide Chemical compound [O-][N+]#N GQPLMRYTRLFLPF-UHFFFAOYSA-N 0.000 description 15
- 230000032683 aging Effects 0.000 description 15
- 239000000758 substrate Substances 0.000 description 14
- 239000003570 air Substances 0.000 description 13
- 239000012876 carrier material Substances 0.000 description 13
- 239000011248 coating agent Substances 0.000 description 12
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 11
- 239000000203 mixture Substances 0.000 description 11
- 229910052757 nitrogen Inorganic materials 0.000 description 11
- 230000001590 oxidative effect Effects 0.000 description 11
- 229910001404 rare earth metal oxide Inorganic materials 0.000 description 11
- 238000012360 testing method Methods 0.000 description 11
- 229910052751 metal Inorganic materials 0.000 description 10
- 239000002184 metal Substances 0.000 description 10
- 229910021536 Zeolite Inorganic materials 0.000 description 9
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 9
- 229910044991 metal oxide Inorganic materials 0.000 description 9
- 150000004706 metal oxides Chemical class 0.000 description 9
- 238000007254 oxidation reaction Methods 0.000 description 9
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 8
- 239000011230 binding agent Substances 0.000 description 8
- 230000003647 oxidation Effects 0.000 description 8
- 239000001272 nitrous oxide Substances 0.000 description 7
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 7
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 7
- 238000000746 purification Methods 0.000 description 7
- 229910001928 zirconium oxide Inorganic materials 0.000 description 7
- 229910000420 cerium oxide Inorganic materials 0.000 description 6
- 230000000694 effects Effects 0.000 description 6
- 150000002739 metals Chemical class 0.000 description 6
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 6
- MMKQUGHLEMYQSG-UHFFFAOYSA-N oxygen(2-);praseodymium(3+) Chemical compound [O-2].[O-2].[O-2].[Pr+3].[Pr+3] MMKQUGHLEMYQSG-UHFFFAOYSA-N 0.000 description 6
- 229910003447 praseodymium oxide Inorganic materials 0.000 description 6
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 5
- 125000004429 atom Chemical group 0.000 description 5
- -1 platinum group metals Chemical class 0.000 description 5
- 238000011144 upstream manufacturing Methods 0.000 description 5
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 4
- 229910052782 aluminium Inorganic materials 0.000 description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 4
- 230000008859 change Effects 0.000 description 4
- 150000001875 compounds Chemical class 0.000 description 4
- 239000000446 fuel Substances 0.000 description 4
- 229930195733 hydrocarbon Natural products 0.000 description 4
- 150000002430 hydrocarbons Chemical class 0.000 description 4
- 229910052746 lanthanum Inorganic materials 0.000 description 4
- PLDDOISOJJCEMH-UHFFFAOYSA-N neodymium(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Nd+3].[Nd+3] PLDDOISOJJCEMH-UHFFFAOYSA-N 0.000 description 4
- 238000006722 reduction reaction Methods 0.000 description 4
- 229910052814 silicon oxide Inorganic materials 0.000 description 4
- IATRAKWUXMZMIY-UHFFFAOYSA-N strontium oxide Chemical compound [O-2].[Sr+2] IATRAKWUXMZMIY-UHFFFAOYSA-N 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 3
- 229910002091 carbon monoxide Inorganic materials 0.000 description 3
- 239000000969 carrier Substances 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 238000013461 design Methods 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 238000011068 loading method Methods 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 230000009467 reduction Effects 0.000 description 3
- 229910052710 silicon Inorganic materials 0.000 description 3
- 239000010703 silicon Substances 0.000 description 3
- 235000012239 silicon dioxide Nutrition 0.000 description 3
- 239000000377 silicon dioxide Substances 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 2
- 239000011149 active material Substances 0.000 description 2
- ZWOQODLNWUDJFT-UHFFFAOYSA-N aluminum lanthanum Chemical compound [Al].[La] ZWOQODLNWUDJFT-UHFFFAOYSA-N 0.000 description 2
- VKJLWXGJGDEGSO-UHFFFAOYSA-N barium(2+);oxygen(2-);titanium(4+) Chemical compound [O-2].[O-2].[O-2].[Ti+4].[Ba+2] VKJLWXGJGDEGSO-UHFFFAOYSA-N 0.000 description 2
- RCFVMJKOEJFGTM-UHFFFAOYSA-N cerium zirconium Chemical compound [Zr].[Ce] RCFVMJKOEJFGTM-UHFFFAOYSA-N 0.000 description 2
- 229910052681 coesite Inorganic materials 0.000 description 2
- 229910052906 cristobalite Inorganic materials 0.000 description 2
- 239000000835 fiber Substances 0.000 description 2
- 239000005431 greenhouse gas Substances 0.000 description 2
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 230000000737 periodic effect Effects 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 229910052682 stishovite Inorganic materials 0.000 description 2
- 239000004408 titanium dioxide Substances 0.000 description 2
- 229910052905 tridymite Inorganic materials 0.000 description 2
- GHOKWGTUZJEAQD-ZETCQYMHSA-N (D)-(+)-Pantothenic acid Chemical compound OCC(C)(C)[C@@H](O)C(=O)NCCC(O)=O GHOKWGTUZJEAQD-ZETCQYMHSA-N 0.000 description 1
- 229910000505 Al2TiO5 Inorganic materials 0.000 description 1
- 241000269350 Anura Species 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- 229910021193 La 2 O 3 Inorganic materials 0.000 description 1
- 229910052777 Praseodymium Inorganic materials 0.000 description 1
- 238000003915 air pollution Methods 0.000 description 1
- 229910000287 alkaline earth metal oxide Inorganic materials 0.000 description 1
- ILRRQNADMUWWFW-UHFFFAOYSA-K aluminium phosphate Chemical class O1[Al]2OP1(=O)O2 ILRRQNADMUWWFW-UHFFFAOYSA-K 0.000 description 1
- GHTGICGKYCGOSY-UHFFFAOYSA-K aluminum silicon(4+) phosphate Chemical class [Al+3].P(=O)([O-])([O-])[O-].[Si+4] GHTGICGKYCGOSY-UHFFFAOYSA-K 0.000 description 1
- 239000012080 ambient air Substances 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000010531 catalytic reduction reaction Methods 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
- 239000011247 coating layer Substances 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 230000001143 conditioned effect Effects 0.000 description 1
- 229910052878 cordierite Inorganic materials 0.000 description 1
- 229910052593 corundum Inorganic materials 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 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 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 239000002657 fibrous material Substances 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- CKHJYUSOUQDYEN-UHFFFAOYSA-N gallium(3+) Chemical compound [Ga+3] CKHJYUSOUQDYEN-UHFFFAOYSA-N 0.000 description 1
- 239000003365 glass fiber Substances 0.000 description 1
- 239000003779 heat-resistant material Substances 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- 229910001387 inorganic aluminate Inorganic materials 0.000 description 1
- 229910052909 inorganic silicate Inorganic materials 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- 229910001711 laumontite Inorganic materials 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- 229910052680 mordenite Inorganic materials 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- KTUFCUMIWABKDW-UHFFFAOYSA-N oxo(oxolanthaniooxy)lanthanum Chemical compound O=[La]O[La]=O KTUFCUMIWABKDW-UHFFFAOYSA-N 0.000 description 1
- 125000004437 phosphorous atom Chemical group 0.000 description 1
- 239000006069 physical mixture Substances 0.000 description 1
- 239000002574 poison Substances 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- AABBHSMFGKYLKE-SNAWJCMRSA-N propan-2-yl (e)-but-2-enoate Chemical compound C\C=C\C(=O)OC(C)C AABBHSMFGKYLKE-SNAWJCMRSA-N 0.000 description 1
- 239000011214 refractory ceramic Substances 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 229910001954 samarium oxide Inorganic materials 0.000 description 1
- 229940075630 samarium oxide Drugs 0.000 description 1
- FKTOIHSPIPYAPE-UHFFFAOYSA-N samarium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[Sm+3].[Sm+3] FKTOIHSPIPYAPE-UHFFFAOYSA-N 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000006104 solid solution Substances 0.000 description 1
- 239000004071 soot Substances 0.000 description 1
- 238000005507 spraying Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 230000001629 suppression Effects 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- 229910001845 yogo sapphire Inorganic materials 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
Classifications
-
- 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
- B01D53/9436—Ammonia
-
- 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]
-
- 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
- B01D53/9463—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts with catalysts positioned on one brick
- B01D53/9468—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts with catalysts positioned on one brick in different layers
-
- 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
- B01D53/9477—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts with catalysts positioned on separate bricks, e.g. exhaust systems
-
- 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
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/02—Boron or aluminium; Oxides or hydroxides thereof
- B01J21/04—Alumina
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/12—Silica and alumina
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01J23/56—Platinum group metals
- B01J23/58—Platinum group metals with alkali- or alkaline earth metals
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/56—Platinum group metals
- B01J23/63—Platinum group metals with rare earths or actinides
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
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- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
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- F01N2570/00—Exhaust treating apparatus eliminating, absorbing or adsorbing specific elements or compounds
- F01N2570/18—Ammonia
Definitions
- the present invention is aimed at an exhaust system for reducing exhaust gases and in particular ammonia emissions in the exhaust system of a predominantly stoichiometrically operated spark ignition engine.
- Spark ignition engines or gasoline engines powered by gasoline or natural gas are cleaned in conventional processes using three-way catalysts (TWC). These are able to simultaneously convert the engine's three main gaseous pollutants, namely hydrocarbons, carbon monoxide and nitrogen oxides, into harmless components.
- Stoichiometric means that, on average, there is as much air available to burn the fuel present in the cylinder as is required for complete combustion.
- the combustion air ratio ⁇ (A/F ratio; air/fuel ratio) relates the air mass m L,tats actually available for combustion to the stoichiometric air mass m L,st : If ⁇ ⁇ 1 (e.g. 0.9) this means “lack of air”, one speaks of a rich exhaust gas mixture, ⁇ > 1 (e.g. 1.1) means “excess air” and the exhaust gas mixture is considered lean designated.
- ⁇ 1.1 means that 10% more air is present than would be necessary for the stoichiometric reaction. The same applies to the exhaust gases from internal combustion engines.
- the catalytically active materials used in the known three-way catalysts are generally platinum group metals, in particular platinum, palladium and rhodium, which are present, for example, on ⁇ -aluminum oxide as a support material.
- three-way catalysts contain oxygen storage materials, for example cerium/zirconium mixed oxides. In the latter, cerium oxide, a rare earth metal oxide, is the fundamental component for oxygen storage. In addition to zirconium oxide and cerium oxide, these materials can contain additional components such as other rare earth metal oxides or alkaline earth metal oxides.
- Oxygen storage materials are made by Application of catalytically active materials such as platinum group metals activates and thus also serves as a carrier material for the platinum group metals.
- Compliance with the strict emission values for ammonia requires the use of a storage material to store NH 3 during the rich operating conditions of the combustion engine, particularly in low and medium temperature ranges. engines, as the ammonia is mainly formed under these exhaust gas conditions. The stored ammonia is then converted during lean operating points by oxidation on a layer containing precious metal and/or as part of an SCR reaction. The aim here is to achieve the lowest possible selectivity to N 2 O.
- a special requirement for the catalysts considered here is the high aging stability of the materials used: In addition to the stability against lean gas conditions, their use in the exhaust system of stoichiometrically operated internal combustion engines also requires that they also be used in the exhaust gas with rich or stoichiometric ric composition are stable under hydrothermal exhaust gas conditions.
- the use of catalysts, which preferentially convert ammonia into nitrogen, has already been discussed, particularly in the diesel sector or for use in lean-burning DI petrol engines (US5120695; EP1892395A1; EP1882832A2; EP1876331A2; WO12135871A1; US2011271664AA; WO1111091 9A1, EP3915679A1).
- ammonia slip catalysts or ASCs for short, has also already been described in the area of LNG gasoline engines (EP24258A1). These catalysts often consist of an SCR catalytically active component and a component that catalyzes the oxidation of ammonia. These catalytic converters are usually located in the underbody at the last point of the exhaust system. If for oxidation of the stored If there are not enough nitrogen oxides in the system, the ammonia can also be converted into nitrogen via the ASC with the oxygen present. As it turns out, the aging stability of ASC catalytic converters also depends largely on their design.
- an exhaust system for reducing the harmful exhaust gas components of internal combustion engines having a first three-way catalytic converter and, on the downstream side, a catalyst for reducing ammonia emissions, which has the following components comprises: - a first component made of zeolites and/or zeotypes for storing ammonia; - a second component of an OSC-free noble metal catalyst; - a third component of an OSC-containing noble metal catalyst, the solution to the problem is achieved relatively easily, but no less surprisingly.
- the system according to the invention is characterized by extremely good performance both in terms of the original exhaust gas components and in terms of NH3 and N2O emissions.
- a first component of the catalyst for reducing ammonia emissions consists of zeolites and/or zeotypes Storage of ammonia.
- those skilled in the art are familiar with the zeolites and zeotypes available for this purpose from the diesel sector.
- zeolites or zeotypes work is based on the fact that they can temporarily store ammonia in operating states of the exhaust gas purification system in which ammonia is produced, for example, by over-reduction of nitrogen oxides via a three-way catalytic converter installed on the upstream side, but this cannot be converted by other conventional three-way catalytic converters, for example due to lack of oxygen or insufficient operating temperatures.
- the ammonia stored in this way can then be removed from storage when the operating state of the exhaust gas purification system changes and subsequently or directly converted, for example when sufficient oxygen or nitrogen oxides are present.
- zeolites and zeotypes are present in the first component of the catalyst to reduce ammonia emissions.
- zeolites or zeotypes can be divided into different classes. Zeolites are then divided, for example, according to their channel system and their framework structure. For example, laumontite and mordenite are classified as zeolites, which have a one-dimensional system of channels. Your channels have no connection with each other. Zeolites with a two-dimensional framework structure are characterized by the fact that their channels are connected to one another in a kind of layered system. A third group has a three-dimensional framework structure with cross-layer connections between the channels.
- zeolites or zeotypes are preferably used [Ch. Baerlocher, WM Meier and DH Olson, Atlas of Zeolite Framework Types, Elsevier, 2001].
- zeolite refers to porous materials with a lattice structure of corner-linked AlO4 and SiO4 tetrahedra according to the general formula (WM Meier, Pure & Appl.
- zeolite therefore comprises a network made up of tetrahedra that encloses channels and cavities.
- zeotype refers to a zeolite-like compound that has the same structural type as a natural one occurring or a synthetically produced zeolite compound, which differs from these in that the corresponding cage structure is not made up exclusively of aluminum and silicon framework atoms.
- the aluminum and/or silicon framework atoms are proportionally replaced by other trivalent, quadrivalent or pentavalent framework atoms such as B(III), Ga(III), Ge(IV), Ti(IV) or P(V) replaced.
- the most common method used in practice is the replacement of aluminum and/or silicon framework atoms by phosphorus atoms, for example in the silicon aluminum phosphates or in the aluminum phosphates, which crystallize in zeolite structure types.
- suitable zeolites come from the group of two-dimensional or three-dimensional zeolites/zeotypes.
- They preferably belong to the structure types ACO, AEI, AEN, AFN, AFT, AFX, ANA, APC, APD, ATT, BEA, BIK, CDO, CHA, DDR, DFT, EAB, EDI, EPI, ERI, ESV, ETL, GIS , GOO, IHW, ITE, ITW, LEV, KFI, MER, MON, NSI, OWE, PAU, PHI, RHO, RTH, SAT, SAV, SIV, THO, TSC, UEI, UFI, VNI, YUG, ZON.
- the zeolites or zeotypes in the car exhaust gas catalytic converter according to the invention are selected from the group AEI, AFT, AFX, CHA, DDR, ERI, ESV, ETL, KFI, LEV, UFI and the corresponding zeotypes of these structural types , such as: SAPO. Mixtures of the same can also be present.
- the use of CHA, FER, LEV and AEI is particularly preferred.
- the aging stability of the zeolites or zeotypes used in the exhaust system of predominantly stoichiometrically burning engines is particularly in focus here, since higher temperatures generally prevail here than in a lean-burning engine.
- the exhaust gas composition is also different compared to lean-burn engine exhaust.
- concentration, in particular of hydrocarbons and carbon monoxide, which arrive at the catalyst according to the invention is, on the one hand, higher than in lean-burn engines and the composition also changes depending on the driving style around the stoichiometric range (rich/lean change).
- the hydrothermal temperature stability of zeolites and zeotypes depends heavily on the SAR value (silica-to-alumina ratio) of the zeolite or the ratio corresponding to this value for zeotypes. The amount of silicon atoms remaining in the framework is then related to the substitution atoms.
- the zeolites have a SAR value of 10 - 50, preferably 12 - 35 and most preferably have 13 – 30.
- the zeotype with the corresponding ratio.
- the zeolite or zeotype used is ion-exchanged with transition metal ions.
- the latter are preferably selected from the group consisting of iron and/or copper. Iron is particularly preferred because it has a less oxidizing effect on ammonia compared to copper.
- the zeolite or zeotype described acts as a catalyst for selective catalytic reduction (SCR) (see WO2008106518A2, WO2017187344A1, US2015290632AA, US2015231617AA, WO2014062949A1, US2015231617AA).
- SCR capability is understood to mean the ability to selectively convert NO x and NH 3 in the lean exhaust gas into nitrogen.
- the metals, such as iron and/or copper, which advantageously occur in the catalyst to reduce ammonia emissions, are present in a certain proportion in the first component. This is 0.4-10, more preferably 0.8-6 and very preferably 1.5-4.8% by weight of the first component.
- the iron and/or copper to aluminum ratio is between 0.15 - 0.8, preferably between 0.2 - 0.5 and most preferably between 0.3 - 0.5 for zeolites.
- a corresponding ratio applies to the exchange places available there.
- the metals are at least partially present in ion-exchanged form in the zeolites or zeotypes.
- ion-exchanged zeolites or zeotypes are already introduced into the first component.
- the zeolites or zeotypes are brought together with, for example, a binder and a solution of the metal ions in a liquid, preferably water, and then dried (preferably by spraying).
- the first component can preferably contain further components, in particular non-catalytically active components, such as binders.
- non-catalytically active components such as binders.
- binders temperature-stable metal oxides that are not or only slightly catalytically active, such as SiO2, Al2O3 and ZrO2, are suitable as binders.
- the expert knows which materials come into question here.
- the proportion of such binders in the first component can, for example, be up to 15% by weight, preferably up to 10% by weight, of the component.
- the binder can also be those specified above have metals.
- Binders are suitable for ensuring stronger adhesion of the coating to a carrier.
- a certain particle size of the metal oxides in the binder is advantageous. This can be adjusted accordingly by an expert.
- the ammonia storage ability or capacity addressed in the context of this invention is given as a quotient of the stored mass of ammonia per liter of catalyst support volume.
- the zeolites or zeotypes should increase the ammonia storage capacity of the exhaust gas purification system to at least 0.25 g of ammonia per liter of carrier volume (measured in the fresh state).
- the storage capacity of the ammonia storage components used should be sufficient for the system to contain between 0.25 and 10.0 g of NH 3 per liter of carrier volume, preferably between 0.5 and 8.0 g of NH 3 per liter of carrier volume and particularly preferably between 0. 5 and 5.0 g NH 3 /liter carrier volume of ammonia can be stored (always based on the fresh state).
- the zeolites or zeotypes are present in sufficient quantities in the catalyst to reduce ammonia emissions. A value of 25 - 350 g/L, preferably 75 - 300 g/L and most preferably 100 - 250 g/L of carrier volume has proven to be the preferred amount.
- the volume of the carrier on which the storage material is located is used as the carrier volume.
- the first component of the ammonia emissions reduction catalyst is associated with the second component of the ammonia emissions reduction catalyst.
- the second component consists of an OSC-free precious metal catalyst.
- Precious metal refers in particular to the platinum group metals platinum, palladium and rhodium.
- OSC means Oxygen Storage Catalyst - oxygen storage catalyst.
- This precious metal catalyst therefore essentially has no function of storing the oxygen in the exhaust gas of the internal combustion engine.
- this component has oxygen storage materials, in particular cerium-zirconium mixed oxides, of less than 20 g/L, preferably less than 10 g/L and most preferably less than 5 g/L carrier volume.
- cerium or cerium-zirconium mixed oxides for example, is considered the storage material, including the doping elements present.
- Corresponding OSC-free precious metal catalysts are capable of operating in the already slightly lean exhaust gas of a predominantly stoichiometric engine Internal combustion engine has an oxidative effect on the substances present (NH3, HC, CO). This component is preferably designed so that it becomes active at correspondingly low temperatures.
- the ammonia stored in the zeolite or zeotype is preferably converted into non-harmful nitrogen via this component.
- the oxidation effect should not be too great, otherwise a certain proportion of the powerful greenhouse gas N2O will be formed from ammonia oxidation.
- the second component in the form of an OSC-free precious metal catalyst therefore contains materials that have an oxidative effect on, among other things, ammonia.
- this component contains a temperature-stable, high-surface metal oxide and at least one noble metal selected from the group rhodium, platinum and palladium.
- the total precious metal content of this component is preferably from 0.015 - 5 g/L, more preferably from 0.035 - 1.8 g/L and particularly preferably from 0.07 - 1.2 g/L carrier volume.
- the precious metals platinum or palladium, or platinum and palladium together, are particularly suitable for use in this component that has an oxidative effect on ammonia.
- the person skilled in the art can preferably choose whether to use the strongly oxidative platinum alone or, if necessary, in conjunction with palladium in the second coating layer. If platinum and/or palladium is used, the former should be in the range of 0.015 - 1.42 g/L, more preferably 0.035 - 0.35 g/L carrier volume in the coating. Palladium can be present in the coating between 0.015 - 1.42 g/L, preferably 0.035 - 0.35 g/L carrier volume. The weight ratio of platinum to palladium should be between 1:0 and 1:5, more preferably 1:0 and 1:4 and most preferably 1:0 and 1:2.
- the noble metals in the second component are usually fixed on one or more temperature-stable, high-surface metal oxides as carrier materials. All materials familiar to those skilled in the art for this purpose can be considered as carrier materials. Such materials are in particular metal oxides with a BET surface area of 30 to 250 m 2 /g, preferably 100 to 200 m 2 /g (determined according to DIN 66132 - latest version on the filing date). Particularly suitable carrier materials for the precious metals are selected from the series consisting of aluminum oxide, doped aluminum oxide, silicon oxide, titanium dioxide and mixed oxides from one or more of these. Doped aluminum oxides are, for example, lanthanum oxide, zirconium oxide, barium oxide and/or titanium oxide-doped aluminum oxides.
- Aluminum oxide or lanthanum-stabilized aluminum oxide is advantageously used, in the latter case lanthanum in amounts of in particular 1 to 10% by weight, preferably 3 to 6% by weight, in each case calculated as La2O3 and based on the weight of the stabilized aluminum oxide. Even in the case of aluminum oxide doped with barium oxide, the proportion of barium oxide is in particular 1 to 10% by weight, preferably 3 to 6% by weight, in each case calculated as BaO and based on the weight of the stabilized aluminum oxide.
- Another suitable carrier material is lanthanum-stabilized aluminum oxide, the surface of which is coated with lanthanum oxide, barium oxide and/or strontium oxide. The second coating preferably comprises at least one aluminum oxide or doped aluminum oxide.
- La-stabilized aluminum oxide with a surface area of 100 to 200 m 2 /g is particularly advantageous in this context.
- Such active aluminum oxide is widely described in the literature and is available on the market.
- the first and second components preferably form an SCR catalyst and a function for oxidizing ammonia to nitrogen (eg WO2008106519A1). In this form they are ammonia oxidation catalysts (AMOX) or ammonia barrier catalysts (ASC). If there are not enough nitrogen oxides in the system to oxidize the stored ammonia, the ammonia can also be converted into nitrogen using the second component with the oxygen present. In both cases, if possible, no ammonia or N2O is released into the environment.
- AMOX ammonia oxidation catalysts
- ASC ammonia barrier catalysts
- the first component and the second component of the catalyst for reducing ammonia emissions can therefore preferably consist of an SCR-active coating paired with a second coating that has an oxidative effect on ammonia.
- they are preferably present at least partially on top of one another on the substrate. It is particularly preferred if both coatings are of the same length and one lies on top of the other on the substrate.
- the OSC-free noble metal catalyst of component two is located as a lower layer under the first component made of zeolites and / or zeotypes for storing ammonia as an upper layer.
- the second component is preferably placed directly on the substrate as a coating. There is preferably no further layer between the first component and the second component (FIG. 2).
- a disadvantage of the known systems for reducing ammonia emissions can be that the transition metals in the SCR component, such as iron and/or copper, become predominantly stoichiometric after a long period of use in the exhaust system operated internal combustion engine tend to diffuse into the ammonia oxidation component and poison it. The result is a lower activity of the SCR and the oxidative component.
- Suitable materials for this layer are, in particular, those selected from the group consisting of aluminum oxide, silicon oxide, titanium oxide, zirconium oxide, zeolites or mixtures thereof.
- Very particularly preferred in this context is a layer made of aluminum oxide or silicon oxide, which is preferably located on the substrate in the same length above the lower layer and under the upper layer.
- the catalyst for reducing ammonia emissions has a third component.
- This consists of a precious metal catalyst containing OSC.
- the noble metals in the OSC-containing noble metal catalyst are preferably selected from the group consisting of palladium or rhodium or platinum, platinum and rhodium, palladium and rhodium or palladium and rhodium and platinum together.
- the third component is preferably a coating equipped with three-way catalytic ability. This particularly preferably has precious metals selected from the group of platinum and rhodium, palladium and rhodium, preferably rhodium alone.
- rhodium is present in the second and/or third component (whether alone or in combination with the other aforementioned noble metals), this should preferably be in the range of 0.035 - 1.0 g/L, more preferably 0.1 - 0. There is 35 g/L carrier volume in the respective component. If palladium and/or platinum are also present in the third component, the ranges mentioned above for these metals apply. Suitable three-way catalytically active coatings are described, for example, in DE102013210270A1, DE102020101876A1, EP3247493A1, EP3727655A1.
- the noble metals in the OSC-containing third component are usually fixed on one or more temperature-stable, high-surface metal oxides as carrier materials.
- carrier materials can be considered as carrier materials.
- Such materials are in particular metal oxides with a BET surface area of 30 to 250 m 2 /g, preferably 100 to 200 m 2 /g (determined according to DIN 66132 - latest version on the filing date).
- Particularly suitable carrier materials for the precious metals are selected from the series consisting of aluminum oxide, doped aluminum oxide, silicon oxide, titanium dioxide and mixed oxides from one or more of these.
- Doped aluminum oxides are, for example, lanthanum oxide, zirconium oxide, barium oxide and/or titanium oxide-doped aluminum oxides.
- Aluminum oxide or lanthanum-stabilized aluminum oxide is advantageously used, in the latter case lanthanum in amounts of in particular 1 to 10% by weight, preferably 3 to 6% by weight, in each case calculated as La 2 O 3 and related based on the weight of the stabilized aluminum oxide. Even in the case of aluminum oxide doped with barium oxide, the proportion of barium oxide is in particular 1 to 10% by weight, preferably 3 to 6% by weight, in each case calculated as BaO and based on the weight of the stabilized aluminum oxide.
- Another suitable carrier material is lanthanum-stabilized aluminum oxide, the surface of which is coated with lanthanum oxide, barium oxide and/or strontium oxide. This component preferably comprises at least one aluminum oxide or doped aluminum oxide.
- La-stabilized aluminum oxide with a surface area of 100 to 200 m 2 /g is particularly advantageous in this context.
- Such active aluminum oxide has been widely described in the literature and is available on the market.
- the third component, according to the invention also has oxygen storage materials - it contains OSC.
- the noble metals are preferably deposited both on the carrier materials and on the oxygen storage materials.
- Modern gasoline engines are operated under conditions with a discontinuous course of the air ratio ⁇ . They are subject in a defined manner to a periodic change in the air ratio ⁇ and thus to a periodic change in oxidizing and reducing exhaust gas conditions. In both cases, this change in the air ratio ⁇ is essential for the exhaust gas purification result.
- oxygen storage materials contained in the catalytic converter compensate for these deviations to a certain extent by absorbing oxygen from the exhaust gas as required or released into the exhaust gas (Catalytic Air Pollution Control, Commercial Technology, R. Heck et al., 1995, p.90).
- the OSC-containing noble metal catalysts (modern three-way catalysts) of the second component therefore contain oxygen storage materials, in particular cerium or Ce/Zr mixed oxides. The mass ratio of cerium oxide to zirconium oxide can vary within wide limits in these mixed oxides.
- cerium/zirconium mixed oxides include one or more rare earth metal oxides and can therefore be referred to as cerium/zirconium/rare earth metal mixed oxides.
- cerium/zirconium mixed oxides that do not contain any rare earth metal oxide.
- the term rare earth metal or rare earth metal oxide in the sense of the present invention does not include cerium or cerium oxide.
- Possible rare earth metal oxides in the cerium/zirconium/rare earth metal mixed oxides are, for example, lanthanum oxide, yttrium oxide, praseodymium oxide, neodymium oxide and/or samarium oxide. Lanthanum oxide, yttrium oxide and/or praseodymium oxide are preferred.
- rare earth metal oxides are lanthana and/or yttrium oxide and very particularly preferred is the joint presence of lanthana and yttrium oxide, yttrium oxide and praseodymium oxide, as well as lanthana and praseodymium oxide in the cerium/zirconium/rare earth metal mixed oxide.
- this noble metal catalyst has two different cerium/zirconium/rare earth metal mixed oxides, preferably one doped with La and Y and one doped with La and Pr.
- the oxygen storage components are preferably free of neodymium oxide.
- the proportion of rare earth metal oxide(s) in the cerium/zirconium/rare earth metal mixed oxides is advantageously 3 to 20% by weight based on the cerium/zirconium/rare earth metal mixed oxide. If the cerium/zirconium/rare earth metal mixed oxides contain yttrium oxide as the rare earth metal, its proportion is preferably 4 to 15% by weight based on the cerium/zirconium/rare earth metal mixed oxide. If the cerium/zirconium/rare earth mixed oxides contain praseodymium oxide as the rare earth metal, its proportion is preferably 2 to 10% by weight based on the cerium/zirconium/rare earth mixed oxide.
- cerium/zirconium/rare earth mixed oxides contain lanthanum oxide and another rare earth oxide as the rare earth metal, such as yttrium oxide or praseodymium oxide, their mass ratio is in particular 0.1 to 1.25, preferably 0.1 to 1.
- the third component usually contains Oxygen storage materials in amounts of 15 to 120 g/l, based on the volume of the wall flow filter substrate.
- the OSC-containing noble metal catalysts therefore have the temperature-stable, high-surface support materials mentioned and, in addition to these, the oxygen-storing materials just explained.
- the mass ratio of temperature-stable, high-surface carrier materials and oxygen storage components in this component is usually 0.25 to 1.5, for example 0.3 to 1.3.
- the weight ratio of the sum of the masses of all support materials, such as aluminum oxides (including doped aluminum oxides) to the sum of the masses of all cerium/zirconium mixed oxides in the OSC-containing noble metal catalyst is 10:90 to 75:25, preferably 20: 80 to 65:35.
- the noble metals can only be deposited on the temperature-stable, high-surface support materials. As already indicated above, it is preferred if the noble metals are deposited both on the carrier materials mentioned and on the oxygen storage materials.
- the OSC-containing precious metal catalyst of the third component is positioned in the exhaust gas line in the exhaust gas direction directly in front of a combination of zeolites or zeotypes for storing ammonia (first component) and OSC-free precious metal catalyst (second component), or the OSC-containing precious metal catalyst is positioned in the exhaust system in the exhaust gas direction directly after a combination of zeolites or zeotypes for storing ammonia and OSC-free precious metal catalyst.
- “After” means accordingly, the fact that one of the components is later contacted with the incoming exhaust gas after the exhaust gas has come into contact with the other component.
- Direct means that there is no further exhaust treatment layer or device between these components. This can preferably be accomplished by either positioning two separate substrates with corresponding coatings directly one behind the other in the exhaust system, or by coating one substrate in a correspondingly zoned manner.
- the first component containing zeolites or zeotypes for storing ammonia is positioned, as already indicated above, in a separate layer on the OSC-free noble metal catalyst (second component) lying on the substrate.
- the third component then forms a zoned arrangement with the double coating of the first and second components, in which the two zones merely touch each other (see FIG.
- the two coatings can also at least partially overlap.
- the first component containing the zeolites or zeotypes for storing ammonia is preferably always positioned on the OSC-free noble metal catalyst.
- the components of the catalyst for reducing ammonia emissions are applied to one or more (see above) supports, preferably to one or more flow-through substrate(s), by a coating step familiar to those skilled in the art (DE102019100099A1 and literature cited there).
- a filter substrate such as a wall flow filter is also possible in this context.
- Flow-through substrates are catalyst supports that are common in the prior art and can consist of metal, for example WO17153239A1, WO16057285A1, WO15121910A1 and literature cited therein) or ceramic materials.
- “Corrugated substrates” can also be viewed as flow-through substrates. These are known to those skilled in the art as carriers made of corrugated sheets, which consist of inert materials. Suitable inert materials are, for example, fibrous materials with an average fiber diameter of 50 to 250 ⁇ m and an average fiber length of 2 to 30 mm. Fibrous, heat-resistant materials made of silicon dioxide, especially glass fibers, are preferred. However, refractory ceramics such as cordierite, silicon carbide or aluminum titanate etc.
- the total amount of coatings in the catalyst to reduce ammonia emissions is selected so that the catalyst according to the invention is used as efficiently as possible overall.
- the total amount of coatings (solids content) per carrier volume (total volume of the carrier) can be between 100 and 600 g/L, in particular between 150 and 400 g/L.
- the third component is preferably used in an amount of 15 to 250 g/L, in particular between 20 and 200 g/L, particularly preferably about 20 - 150 g/L of carrier volume.
- the first component is preferably used in an amount of 50 to 350 g/L, in particular between 120 and 250 g/L, particularly preferably about 145 - 230 g/L of carrier volume.
- the second component is preferably used from 50 to 350 g/L, in particular between 120 and 250 g/L, particularly preferably from about 145 - 230 g/L carrier volume.
- the present exhaust system has a first three-way catalyst and a catalyst positioned downstream to reduce ammonia emissions.
- the first three-way catalyst can have the same components as the OSC-containing noble metal catalyst of the second component.
- the first catalyst with three-way activity has, in a further preferred embodiment, a 2-layer structure with two different three-way coatings, preferably as described in EP3247493A1.
- Downstream refers to the fact that the exhaust gas flow first hits the upstream catalytic converter and then the downstream catalytic converter. The reverse applies to the upstream side.
- Euro 7 legislation it has proven to be advantageous if an exhaust system for a predominantly stoichiometric engine has a unit for filtering small soot and ash particles.
- GPF are gasoline particle filters and are well known to those skilled in the art (EP3737491A1, EP3601755A1).
- An exhaust gas design is particularly preferred in which the first three-way catalytic converter and the GPF on the downstream side are installed in a housing close to the engine if necessary. Close to the engine in the sense of the invention refers to an area in the exhaust system that is in a position close to the engine, i.e. approx. 10 - 80 cm, preferably 20 - 60 cm away from the engine outlet.
- the catalytic converter is installed last in the exhaust direction in the underbody of a vehicle to reduce ammonia emissions, so that the exhaust gas is then released into the ambient air.
- the exhaust system can also have additional exhaust units such as additional three-way catalytic converters or hydrocarbon storage (HC traps) or nitrogen oxide storage (LNT).
- the underbody is the area below the driver's cab.
- TWC three-way catalytic converter
- This three-way catalyst is preferably one as described in the prior art (DE102013210270A1, DE102020101876A1, EP3247493A1, EP3727655A1). Zoned or layered versions are now the norm for TWCs.
- at least one of the additional catalysts with three-way activity has a 2-layer structure with two different three-way coatings, preferably as described in EP3247493A1.
- the at least second three-way catalytic converter just described in the exhaust system according to the invention can be installed in the underbody of the vehicle, but it can also be in a position close to the engine.
- the range of possible Euro 7 systems is large.
- the catalyst for reducing ammonia emissions is preferably located last in the underbody and in fluid communication with the further catalyst or catalysts or the filter of the car exhaust system.
- the car exhaust system preferably has no additional injection device for ammonia or a precursor compound for ammonia.
- the present invention relates to a method for reducing harmful exhaust gas components from predominantly stoichiometrically operated internal combustion engines, in particular spark-ignited gasoline engines, in which the exhaust gas is directed via an exhaust system according to the invention. It should be noted that the preferred embodiments of the car exhaust system also apply mutatis mutandis to the present method.
- the present invention is directed to an exhaust gas purification system, in particular for stoichiometrically operated internal combustion engines.
- Fig.1 Chart to explain the measurement of ammonia storage capacity.
- Fig.2 Catalyst for reducing ammonia emissions with the first component (1), the second component (2) and the third component (3).
- Fig.3 Representation of the different combinations of a TWC with an SCR or ASC
- Fig.4 Emission values in comparison
- Fig.5 Exhaust system according to the invention with a three-way catalytic converter (A) close to the engine, a GPF close to the engine and the following catalytic converter to reduce ammonia emissions.
- nen (C) Exhaust system according to the invention with a three-way catalytic converter (A) close to the engine, a GPF close to the engine and the following catalytic converter to reduce ammonia emissions.
- nen C
- A. Determination of the ammonia storage capacity This is determined experimentally in a flow tube reactor. To avoid undesirable ammonia oxidation on the reactor material, a reactor made of quartz glass is used. A drill core is taken as a test specimen from the area of the catalytic converter whose ammonia storage capacity is to be determined. A drill core with a diameter of 1 inch and a length of 3 inches is preferably taken as a test specimen. The drill core is inserted into the flow tube reactor and at a temperature of 600 ° C in a gas atmosphere consisting of 500 ppm nitrogen monoxide, 5 vol.% oxygen, 5 vol.% water and the rest nitrogen with a space velocity of 30000 h -1 for 10 minutes conditioned.
- the measuring temperature of 200 °C is then reached in a gas mixture of 0 vol.% oxygen, 5 vol.% water and the rest nitrogen at a space velocity of 30,000 h -1 .
- the NH 3 storage phase is initiated by switching on a gas mixture of 450 ppm ammonia, 0 vol.% oxygen, 5 vol.% water and the rest nitrogen at a space velocity of 30,000 h -1 .
- This gas mixture remains switched on until a stationary ammonia breakthrough concentration is recorded on the downstream side of the test specimen.
- the mass of ammonia stored on the test specimen is calculated from the recorded ammonia breakthrough curve by integration from the start of the NH 3 storage phase until stationarity is reached, taking into account the measured stationary NH 3 breakthrough concentration and the known volume flow (hatched area in Figure 1).
- the ammonia storage capacity is calculated as the quotient of the stored mass of ammonia divided by the volume of the tested core.
- B. Preparation of the precious metal-containing coatings with TWC activity A conventional double-layer TWC with a high content of oxygen storage component and a noble metal loading of 20 g/ft 3 Pd and 5 g/ft 3 Rh was coated on a support.
- C. Production of the SCR coatings A commercially available iron SCR technology was coated on a carrier.
- the aging consists of fuel cut-off aging with an exhaust gas temperature of 950 °C in front of the inlet of the TWC near the engine (maximum bed temperature 1030 °C).
- the aging period and the inlet temperature for the catalytic converter in the underbody position are specified individually for each test.
- Test conditions The different catalytic converters were tested in the underbody position on a highly dynamic engine test bench in a WLTC driving cycle. Here, a series-produced TWC containing Pd/Rh was placed in an aged state in a position close to the engine.
- NH 3 emissions refers to the NH 3 emissions of a system with one of the catalytic converters shown in the underbody position over the entire driving cycle in relation to the emissions of the corresponding system in the absence of a catalytic converter in underbody position.
- Table 1 shows the temperatures at which the catalysts show 50% conversion for hydrocarbons, carbon monoxide and nitrogen oxides in a light-off test after fuel-cut aging in the underbody position. A lower T 50 value corresponds to a higher catalytic activity. A catalytic converter containing only rhodium shows the best starting behavior in this test. Tab.1:
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Abstract
La présente invention concerne un système de gaz d'échappement permettant de réduire les émissions de gaz d'échappement et en particulier les émissions d'ammoniac dans le train d'échappement d'un moteur à allumage par étincelle fonctionnant principalement de manière stœchiométrique.
Applications Claiming Priority (16)
Application Number | Priority Date | Filing Date | Title |
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DE102022108768.9 | 2022-04-11 | ||
DE102022108768 | 2022-04-11 | ||
DE102022119441.8 | 2022-08-03 | ||
DE102022119443.4 | 2022-08-03 | ||
DE102022119442.6 | 2022-08-03 | ||
DE102022119443 | 2022-08-03 | ||
DE102022119441 | 2022-08-03 | ||
DE102022119442 | 2022-08-03 | ||
DE102023101772.1A DE102023101772A1 (de) | 2022-04-11 | 2023-01-25 | Abgassystem für überwiegend stöchiometrisch betriebene Verbrennungsmotoren aufweisend einen Katalysator zur Verminderung der Ammoniakemissionen |
DE102023101772.1 | 2023-01-25 | ||
DE102023101779.9 | 2023-01-25 | ||
DE102023101768.3A DE102023101768A1 (de) | 2022-04-11 | 2023-01-25 | Abgassystem für überwiegend stöchiometrisch betriebene Verbrennungsmotoren aufweisend einen Katalysator zur Verminderung der Ammoniakemissionen |
DE102023101768.3 | 2023-01-25 | ||
DE102023101763.2A DE102023101763A1 (de) | 2022-04-11 | 2023-01-25 | Abgassystem für überwiegend stöchiometrisch betriebene Verbrennungsmotoren aufweisend einen Katalysator zur Verminderung der Ammoniakemissionen |
DE102023101779.9A DE102023101779A1 (de) | 2022-04-11 | 2023-01-25 | Abgassystem für überwiegend stöchiometrisch betriebene Verbrennungsmotoren aufweisend einen Katalysator zur Verminderung der Ammoniakemissionen |
DE102023101763.2 | 2023-01-25 |
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PCT/EP2023/059083 WO2023198574A1 (fr) | 2022-04-11 | 2023-04-06 | Système de gaz d'échappement pour moteurs à combustion interne principalement à fonctionnement stœchiométrique, comprenant un catalyseur pour réduire les émissions d'ammoniac |
PCT/EP2023/059082 WO2023198573A1 (fr) | 2022-04-11 | 2023-04-06 | Système de gaz d'échappement pour moteurs à combustion interne à fonctionnement principalement stœchiométrique, comprenant un catalyseur pour réduire les émissions d'ammoniac |
PCT/EP2023/059079 WO2023198570A1 (fr) | 2022-04-11 | 2023-04-06 | Système de gaz d'échappement pour moteurs à allumage par étincelle fonctionnant principalement de manière stœchiométrique, comprenant un catalyseur permettant de réduire les émissions d'ammoniac |
PCT/EP2023/059081 WO2023198572A1 (fr) | 2022-04-11 | 2023-04-06 | Système de gaz d'échappement pour moteurs à combustion interne principalement à fonctionnement stoechiométrique, comprenant un catalyseur pour réduire les émissions d'ammoniac |
PCT/EP2023/059084 WO2023198575A1 (fr) | 2022-04-11 | 2023-04-06 | Système de gaz d'échappement pour moteurs à combustion interne à fonctionnement principalement stœchiométrique, comprenant un catalyseur pour réduire les émissions d'ammoniac |
PCT/EP2023/059078 WO2023198569A1 (fr) | 2022-04-11 | 2023-04-06 | Catalyseur de blocage d'ammoniac pour moteurs à combustion interne stoechiométrique |
PCT/EP2023/059080 WO2023198571A1 (fr) | 2022-04-11 | 2023-04-06 | Système de gaz d'échappement pour moteurs à combustion interne à fonctionnement principalement stœchiométrique, comprenant un catalyseur pour réduire les émissions d'ammoniac |
PCT/EP2023/059087 WO2023198577A1 (fr) | 2022-04-11 | 2023-04-06 | Système de gaz d'échappement pour moteurs à combustion interne fonctionnant principalement de manière stœchiométrique, comprenant un catalyseur pour réduire les émissions d'ammoniac |
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PCT/EP2023/059082 WO2023198573A1 (fr) | 2022-04-11 | 2023-04-06 | Système de gaz d'échappement pour moteurs à combustion interne à fonctionnement principalement stœchiométrique, comprenant un catalyseur pour réduire les émissions d'ammoniac |
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PCT/EP2023/059084 WO2023198575A1 (fr) | 2022-04-11 | 2023-04-06 | Système de gaz d'échappement pour moteurs à combustion interne à fonctionnement principalement stœchiométrique, comprenant un catalyseur pour réduire les émissions d'ammoniac |
PCT/EP2023/059078 WO2023198569A1 (fr) | 2022-04-11 | 2023-04-06 | Catalyseur de blocage d'ammoniac pour moteurs à combustion interne stoechiométrique |
PCT/EP2023/059080 WO2023198571A1 (fr) | 2022-04-11 | 2023-04-06 | Système de gaz d'échappement pour moteurs à combustion interne à fonctionnement principalement stœchiométrique, comprenant un catalyseur pour réduire les émissions d'ammoniac |
PCT/EP2023/059087 WO2023198577A1 (fr) | 2022-04-11 | 2023-04-06 | Système de gaz d'échappement pour moteurs à combustion interne fonctionnant principalement de manière stœchiométrique, comprenant un catalyseur pour réduire les émissions d'ammoniac |
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WO2023198575A1 (fr) | 2023-10-19 |
WO2023198573A1 (fr) | 2023-10-19 |
WO2023198577A1 (fr) | 2023-10-19 |
WO2023198572A1 (fr) | 2023-10-19 |
WO2023198571A1 (fr) | 2023-10-19 |
WO2023198569A1 (fr) | 2023-10-19 |
WO2023198574A1 (fr) | 2023-10-19 |
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