JP2019529069A - ルテニウム含浸セリア触媒 - Google Patents
ルテニウム含浸セリア触媒 Download PDFInfo
- Publication number
- JP2019529069A JP2019529069A JP2019504887A JP2019504887A JP2019529069A JP 2019529069 A JP2019529069 A JP 2019529069A JP 2019504887 A JP2019504887 A JP 2019504887A JP 2019504887 A JP2019504887 A JP 2019504887A JP 2019529069 A JP2019529069 A JP 2019529069A
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- Prior art keywords
- composition
- catalyst
- adsorption
- exhaust gas
- low temperature
- Prior art date
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Links
- 229910052707 ruthenium Inorganic materials 0.000 title claims abstract description 26
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 title claims abstract description 18
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 title claims abstract description 18
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 title claims abstract description 18
- 239000003054 catalyst Substances 0.000 title claims description 231
- 239000000203 mixture Substances 0.000 claims abstract description 225
- 229910052751 metal Inorganic materials 0.000 claims abstract description 72
- 239000002184 metal Substances 0.000 claims abstract description 71
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- 150000004706 metal oxides Chemical class 0.000 claims abstract description 61
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- 238000011068 loading method Methods 0.000 claims description 17
- 238000002485 combustion reaction Methods 0.000 claims description 12
- 229910052788 barium Inorganic materials 0.000 claims description 9
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 claims description 9
- 150000002500 ions Chemical class 0.000 claims description 9
- 239000010457 zeolite Substances 0.000 claims description 9
- 229910021536 Zeolite Inorganic materials 0.000 claims description 7
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 7
- 229910001404 rare earth metal oxide Inorganic materials 0.000 claims description 6
- 239000000919 ceramic Substances 0.000 claims description 4
- 239000007789 gas Substances 0.000 abstract description 114
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 abstract description 27
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- 238000006243 chemical reaction Methods 0.000 description 10
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 10
- 150000002739 metals Chemical class 0.000 description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 9
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- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 7
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 7
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 7
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- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 6
- 238000001035 drying Methods 0.000 description 6
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- 229910052688 Gadolinium Inorganic materials 0.000 description 5
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 5
- 229910052777 Praseodymium Inorganic materials 0.000 description 5
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- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 4
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 4
- 229910052779 Neodymium Inorganic materials 0.000 description 4
- 229910010413 TiO 2 Inorganic materials 0.000 description 4
- 238000004833 X-ray photoelectron spectroscopy Methods 0.000 description 4
- 239000001569 carbon dioxide Substances 0.000 description 4
- 229910002092 carbon dioxide Inorganic materials 0.000 description 4
- 238000002474 experimental method Methods 0.000 description 4
- 239000010948 rhodium Substances 0.000 description 4
- 239000000377 silicon dioxide Substances 0.000 description 4
- 229910052692 Dysprosium Inorganic materials 0.000 description 3
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- 229910052693 Europium Inorganic materials 0.000 description 3
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- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 description 3
- 229910052772 Samarium Inorganic materials 0.000 description 3
- 229910052771 Terbium Inorganic materials 0.000 description 3
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- 230000008901 benefit Effects 0.000 description 3
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- 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
- 229910052746 lanthanum Inorganic materials 0.000 description 3
- 229910052759 nickel Inorganic materials 0.000 description 3
- 229910052763 palladium Inorganic materials 0.000 description 3
- 230000008929 regeneration Effects 0.000 description 3
- 238000011069 regeneration method Methods 0.000 description 3
- 150000003839 salts Chemical class 0.000 description 3
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- 229910052727 yttrium Inorganic materials 0.000 description 3
- 229910052845 zircon Inorganic materials 0.000 description 3
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 2
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 2
- 229910021193 La 2 O 3 Inorganic materials 0.000 description 2
- 229910052765 Lutetium Inorganic materials 0.000 description 2
- 229910002651 NO3 Inorganic materials 0.000 description 2
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 2
- 229910052581 Si3N4 Inorganic materials 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 2
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 2
- 230000009471 action Effects 0.000 description 2
- 229910052782 aluminium Inorganic materials 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- VXAUWWUXCIMFIM-UHFFFAOYSA-M aluminum;oxygen(2-);hydroxide Chemical compound [OH-].[O-2].[Al+3] VXAUWWUXCIMFIM-UHFFFAOYSA-M 0.000 description 2
- 239000002280 amphoteric surfactant Substances 0.000 description 2
- 125000000129 anionic group Chemical group 0.000 description 2
- 239000012298 atmosphere Substances 0.000 description 2
- 239000004202 carbamide Substances 0.000 description 2
- 125000002091 cationic group Chemical group 0.000 description 2
- 229910010293 ceramic material Inorganic materials 0.000 description 2
- 239000003638 chemical reducing agent Substances 0.000 description 2
- 229910052804 chromium Inorganic materials 0.000 description 2
- 239000011651 chromium Substances 0.000 description 2
- 239000000356 contaminant Substances 0.000 description 2
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- 239000010949 copper Substances 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 230000003247 decreasing effect Effects 0.000 description 2
- KZHJGOXRZJKJNY-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Si]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O KZHJGOXRZJKJNY-UHFFFAOYSA-N 0.000 description 2
- 238000010304 firing Methods 0.000 description 2
- 239000012530 fluid Substances 0.000 description 2
- 229910052741 iridium Inorganic materials 0.000 description 2
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- 239000007788 liquid Substances 0.000 description 2
- 239000000395 magnesium oxide Substances 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
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- 238000002360 preparation method Methods 0.000 description 2
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- 229910052703 rhodium Inorganic materials 0.000 description 2
- 229910052710 silicon Inorganic materials 0.000 description 2
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 2
- 239000003381 stabilizer Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 239000004094 surface-active agent Substances 0.000 description 2
- 239000000725 suspension Substances 0.000 description 2
- 239000002562 thickening agent Substances 0.000 description 2
- 239000010936 titanium Substances 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- DUFCMRCMPHIFTR-UHFFFAOYSA-N 5-(dimethylsulfamoyl)-2-methylfuran-3-carboxylic acid Chemical compound CN(C)S(=O)(=O)C1=CC(C(O)=O)=C(C)O1 DUFCMRCMPHIFTR-UHFFFAOYSA-N 0.000 description 1
- 229910000505 Al2TiO5 Inorganic materials 0.000 description 1
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229910001200 Ferrotitanium Inorganic materials 0.000 description 1
- 238000005033 Fourier transform infrared spectroscopy Methods 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 1
- 230000010718 Oxidation Activity Effects 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 230000000274 adsorptive effect Effects 0.000 description 1
- 229910000323 aluminium silicate Inorganic materials 0.000 description 1
- HEHRHMRHPUNLIR-UHFFFAOYSA-N aluminum;hydroxy-[hydroxy(oxo)silyl]oxy-oxosilane;lithium Chemical compound [Li].[Al].O[Si](=O)O[Si](O)=O.O[Si](=O)O[Si](O)=O HEHRHMRHPUNLIR-UHFFFAOYSA-N 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 239000000908 ammonium hydroxide Substances 0.000 description 1
- APUPEJJSWDHEBO-UHFFFAOYSA-P ammonium molybdate Chemical compound [NH4+].[NH4+].[O-][Mo]([O-])(=O)=O APUPEJJSWDHEBO-UHFFFAOYSA-P 0.000 description 1
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- 239000011609 ammonium molybdate Substances 0.000 description 1
- 229940010552 ammonium molybdate Drugs 0.000 description 1
- 239000003945 anionic surfactant Substances 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
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- 238000010438 heat treatment Methods 0.000 description 1
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- 230000007774 longterm Effects 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
- 239000000391 magnesium silicate Substances 0.000 description 1
- 229910052919 magnesium silicate Inorganic materials 0.000 description 1
- 235000019792 magnesium silicate Nutrition 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 229910001092 metal group alloy Inorganic materials 0.000 description 1
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 1
- 238000003801 milling Methods 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 239000002736 nonionic surfactant Substances 0.000 description 1
- 229910052762 osmium Inorganic materials 0.000 description 1
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 description 1
- 235000006408 oxalic acid Nutrition 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
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- 239000006069 physical mixture Substances 0.000 description 1
- 239000010970 precious metal Substances 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
- 239000011819 refractory material Substances 0.000 description 1
- 239000003870 refractory metal Substances 0.000 description 1
- 238000000518 rheometry Methods 0.000 description 1
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
- GTCKPGDAPXUISX-UHFFFAOYSA-N ruthenium(3+);trinitrate Chemical compound [Ru+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O GTCKPGDAPXUISX-UHFFFAOYSA-N 0.000 description 1
- YBCAZPLXEGKKFM-UHFFFAOYSA-K ruthenium(iii) chloride Chemical compound [Cl-].[Cl-].[Cl-].[Ru+3] YBCAZPLXEGKKFM-UHFFFAOYSA-K 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 description 1
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
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- 239000010935 stainless steel Substances 0.000 description 1
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- 229910052720 vanadium Inorganic materials 0.000 description 1
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 description 1
- 239000011800 void material Substances 0.000 description 1
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Images
Classifications
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
- F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
- F01N3/0807—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by using absorbents or adsorbents
- F01N3/0828—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by using absorbents or adsorbents characterised by the absorbed or adsorbed substances
- F01N3/0842—Nitrogen oxides
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
- B01D53/9404—Removing only nitrogen compounds
- B01D53/9409—Nitrogen oxides
- B01D53/9413—Processes characterised by a specific catalyst
- B01D53/9422—Processes characterised by a specific catalyst for removing nitrogen oxides by NOx storage or reduction by cyclic switching between lean and rich exhaust gases (LNT, NSC, NSR)
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/02—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 by adsorption, e.g. preparative gas chromatography
- B01D53/04—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 by adsorption, e.g. preparative gas chromatography with stationary adsorbents
- B01D53/0407—Constructional details of adsorbing systems
-
- 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
- B01D53/9481—Catalyst preceded by an adsorption device without catalytic function for temporary storage of contaminants, e.g. during cold start
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Abstract
Description
本発明の低温NOx吸着体(LT−NA)組成物は、活性金属を含浸させた金属酸化物担体を含み、活性金属の大半はルテニウムである。本明細書において、ルテニウムが「大半」であるとは、存在する活性金属の総量に対するルテニウムの量が少なくとも50質量%であることを意味する。本明細書で使用される「活性金属」は、白金族金属またはその酸化物を意味し、白金(Pt)、パラジウム(Pd)、ルテニウム(Ru)、ロジウム(Rh)、オスミウム(Os)、イリジウム(Ir)およびそれらの混合物が例として挙げられる。ルテニウム活性金属の濃度は変化し得るが、通常、含浸させた金属酸化物担体の総質量に対し約0.01質量%から約5質量%である。いくつかの実施形態において、NOx吸着体組成物は、あらゆる追加の活性金属を実質的に含まない。本明細書で使用される「追加の活性金属を実質的に含まない」という表現は、NOx吸着体組成物に意図的に添加される追加の活性金属がなく、かつNOx吸着体組成物中に存在する追加の活性金属の質量百分率は約0.01質量%未満であることを意味する。
1つまたは複数の実施形態によると、低温NOx吸着体組成物の基材キャリアは、自動車触媒の製造に一般的に使用される任意の材料から構成され得、通常、金属またはセラミックのハニカム構造を含む。通常、基材は、ウォッシュコート組成物が塗布され、かつ付着する複数の壁面を提供し、それによって触媒組成物の基材キャリアとして働く。
通常、活性金属含浸金属酸化物担体の製造は、粒子形態の金属酸化物担体に、ルテニウム前駆体溶液といった活性金属溶液を含浸させる工程を含む。インシピエントウェットネス技術を使用し、同一の担体粒子または別々の担体粒子に活性金属を含浸させることができる。
活性金属含浸金属酸化物担体を含有するキャリア粒子の形態である上記の触媒組成物は、水と混合され、ハニカム型基材といった触媒基材キャリアを被覆するためのスラリーを形成する。
従来のリーンNOxトラップ(LNT)システムにおいて、NOx吸着体は、NOxを貯留するための塩基性収着剤成分(例えばCeO2またはBaO)、およびNOを触媒的に酸化(例えばPt)および還元(例えばRh)するための白金族金属を含有する。従来のLTN触媒は、式1〜6に示されるようにエンジン出口のNOがN2へ転化される、周期的なリーン(捕集モード)およびリッチ(再生モード)排気条件下で作用する。
2NO+O2→2NO2 (1)
4NO2+2MCO3+O2→2M(NO3)2+2CO2 (2)
リッチ条件(再生モード):
M(NO3)2+2CO→MCO3+NO2+NO+CO2 (3)
NO2+CO→NO+CO2 (4)
2NO+2CO→N2+2CO2 (5)
2NO+2H2→N2+2H2O (6)
本発明の排出ガス処理システムは、ディーゼルエンジンまたはリーンバーンガソリンエンジンからの排気ガス排出物を処理するための、ディーゼル酸化触媒(DOC)、低温NOx吸着体(LT−NA)および/または選択的触媒還元(SCR)触媒といった成分を、1種または複数種含む。排出物処理システムにおける各種成分の相対的配置は変化し得るが、排出物処理システムは、煤煙フィルタ成分および/または追加の触媒成分をさらに含んでもよい。
本発明の特定の態様を説明するために記載され、それらに限定されると解釈されない以下の実施例によって、本発明の態様をより十分に説明する。
粉末試料の多くは、以下の手順に従って同様に製造した:
キャリア材料(CeO2、Al2O3、TiO2など)に水を添加して固形分30%のスラリーとし、90%粒子径が15μm未満になるまでスラリーをミル処理した。ミル処理されたキャリアスラリーの一部を採取し、所望の負荷量に応じた適切な濃度の金属前駆体溶液を添加した。混合物を攪拌しながら乾燥させ、空気中、450℃で2時間焼成し、粉砕し、かつふるい分けし、平均粒子径が約500〜1000□mの焼成粉末を作製した。焼成粉末を、10%蒸気中、600℃で12時間エージングした。
1.Ru(NO)、Pd、Rh、Cu、Ni、Ag、Feの硝酸塩前駆体
2.シュウ酸Sn
3.モリブデン酸アンモニウム
4.Ptアンミン錯体
反応器を通る流れに対して粉末触媒の吸着および放出実験を実施した。実施例1で得られた各粉末(500〜1000μm)3グラムを試験に用いた。供給ガス組成物は、流速750L/時で、NO250ppm、NO250ppm、CO150ppm、C3H650ppm、O210%、H2O10%、残部のN2からなった。
図7に示されるように、NOおよびNO2の吸着について、実施例1で製造された2%Ru/CeO2粉末触媒を純粋なCeO2と比較した。入口におけるNOおよびNO2の濃度は、それぞれ250ppmおよび50ppmであった。2%Ru/CeO2試料が示した試験開始時におけるNOおよびNO2の吸着は、ほぼ100%であった。NOの吸着は温度が上昇するにつれて徐々に減少したが、NO2の破過は300℃を超えるまで見られなかった。一方、純粋なCeO2上に吸着したNOは、試験開始時においてわずか約25%であった。NO2の吸着はより強力であったが、NO2の最初の破過は200℃付近で観測された。NO/NO2濃度が入口濃度を上回ると、放出が開始した。2%Ru/CeO2試料は、2個の放出ピーク:200℃付近に1個のショルダーピーク、および260℃付近に1個の強いピークを有した。より低い温度における放出ピークは、純粋なCeO2で観測された単一の放出ピークと同様であった。Ru/CeO2に特有な別の特徴は、NO濃度の減少およびNO2濃度の上昇から明らかであるように、NOからNO2への酸化が300℃を超える温度で観測された点であった。純粋なCeO2は、NOの酸化に対し、いかなる活性も示さなかった。
2%Ruに対する異なるキャリア材料の影響を評価し、結果を表1に示す。最も高いNOx吸着%はCeO2で観測され、次に高いNOx吸着はZrO2担体上で観測され、CeO2の40%未満であった。高い水熱安定性を有するドープCeO2材料(OSC)は、NOx吸着においていかなる利点ももたらさなかった。
Ru以外のある範囲の金属の影響を表3および表4に示す。データを2つの群に分類し、1つの群(表3)は、同じ質量%負荷量で金属を含有し、NO/NO2供給流を用いて試験し、他の群(表4)は、異なる質量%の負荷量だが同じモル%負荷量で金属を含有し、NOのみの供給流を用いて試験した。いずれの条件下においても、Ru/CeO2試料は、はるかに高いNOx吸着効率を示した。
純粋なCeO2、または異なる酸化物を2〜30質量%の負荷量でドープしたCeO2上に2質量%のRuを堆積させた。NOx吸着の結果を表5に示す。データは、5%以上のSi、NdおよびZr酸化物ならびに10%Pr酸化物は、より低いNOx吸着容量をもたらしたことを明らかに示す。
NOx吸着に対するRu濃度(0.5%から5%)の影響を評価し、結果を表6に示す。Ru0.5%から3%でNOx吸着にわずかな増加が観測され、その後さらにRu負荷量を増加させると緩やかな減少傾向が確認された。
比較試料:ベーマイトアルミナ粉末をDI水へ攪拌しながら添加することによりアルミナバインダ希釈溶液(全固形分5%)を製造した。均一な溶液が得られた後、CeO2キャリアを添加し、固形分が約50%のスラリー懸濁液を形成させた。1:1wt/wtHNO3を用いてスラリーのpHをpH4〜5に調整し、最終粒子径D90が12〜15μmに達するまでミル処理を行った。次いで、400/4ハニカム基材上に固形分42〜46%のスラリーを塗布した。乾燥後、触媒を、空気中、590℃で1時間焼成した。結果として得られたウォッシュコート負荷量は2.0g/in3であった。
Euro VIで校正された高負荷ディーゼルエンジンに基づく排気条件を使用し、過渡ディーゼル条件下でモノリス触媒を試験した。6回の冷間始動WHTC反復試験を通して触媒を評価した。NO、NO2およびNOxの濃度を、触媒出口のFTIR検出器によって同時に観察した。以下の検討において示されるデータは、5回目のサイクルで得られた。未被覆のモノリス基材をブランク実験に使用した。
Claims (23)
- 活性金属および金属酸化物担体を含む低温NOx吸着体組成物であって、金属酸化物担体は、NOx吸着体組成物の総質量に対して50質量%を超えるセリアを含み、活性金属は、NOx吸着体組成物の総質量に対して約0.01質量%から約5質量%のルテニウムを含む、低温NOx吸着体組成物。
- バリウムまたはゼオライトを実質的に含まない、請求項1に記載の低温NOx吸着体組成物。
- 金属酸化物担体が、NOx吸着体の総質量に対して90質量%を超えるセリアを含む、請求項1に記載の低温NOx吸着体組成物。
- 金属酸化物担体が、少なくとも1種の追加の金属酸化物を含み、少なくとも1種の追加の金属酸化物が、希土類金属酸化物である、請求項1に記載の低温NOx吸着体組成物。
- 金属酸化物担体が、Pr6O11、ZrO2、Gd2O3およびそれらの組合せから選択される少なくとも1種の追加の金属酸化物を含む、請求項1に記載の低温NOx吸着体組成物。
- 少なくとも1種の追加の金属酸化物が、NOx吸着体組成物の総質量に対して約0.1質量%から約10質量%の量で存在する、請求項5に記載の低温NOx吸着体組成物。
- NOx吸着体組成物を構成する活性Ruイオンの表面濃度が、NOx吸着体組成物の総質量に対して少なくとも0.5質量%である、請求項1に記載の低温NOx吸着体組成物。
- NOx吸着体組成物が、排気ガス流から、排気ガス流中に存在するNOの総量に対して少なくとも30〜60質量%の量のNOを、約50℃から約200℃の温度で吸着する、請求項1に記載の低温NOx吸着体組成物。
- NOx吸着体組成物が、約300℃から約600℃の範囲の温度で、排気ガス流中に存在するNOをNO2へ酸化させる、請求項1に記載の低温NOx吸着体組成物。
- NOx吸着体組成物が、約170℃から約300℃の温度で、NOx吸着体組成物に吸着したNOの総量に対して少なくとも55から約100質量%の量のNOを排気ガス流中へ放出し戻す、請求項1に記載の低温NOx吸着体組成物。
- NOx吸着体組成物が、あらゆる追加の活性金属を実質的に含まない、請求項1に記載の低温NOx吸着体組成物。
- NOx吸着体組成物が、リーンNOxトラップに含まれる、請求項1に記載の低温NOx吸着体組成物。
- ガス流に適合した複数のチャネルを有する触媒基材キャリア、および各チャネルを通過する排気ガスと接触するよう位置付けされる、請求項1から12のいずれか一項に記載の低温NOx吸着体組成物を含む触媒物品。
- 基材キャリアが、金属ハニカムまたはセラミックハニカムである、請求項13に記載の触媒物品。
- ハニカムが、ウォールフロー型フィルタ基材またはフロースルー型基材である、請求項14に記載の触媒物品。
- 低温NOx吸着体組成物が、少なくとも約0.5g/in3の負荷量で基材キャリアに塗布される、請求項14に記載の触媒物品。
- 活性金属が、約10から約200g/ft3の量で存在する、請求項13に記載の触媒物品。
- 第2の触媒組成物をさらに含み、第2の触媒組成物が、DOC触媒組成物またはLNT触媒組成物を含み、
第2の触媒組成物が、NOx吸着体触媒組成物を有する基材キャリア上に積層されるかまたは区画される、請求項12に記載の触媒物品。 - 第2の触媒組成物が、基材キャリア上に直接配置される、請求項18に記載の触媒物品。
- 請求項1から12のいずれか一項に記載の低温NOx吸着体組成物、および内燃エンジンの下流に配置されるSCR触媒を含む排気ガス処理システム。
- 低温NOx吸着体組成物が、SCR触媒の上流に位置する基材キャリア上に存在する、請求項20に記載の排気ガス処理システム。
- 低温NOx吸着体組成物およびSCR触媒が、同一の基材キャリア上に配置される、請求項20に記載の排気ガス処理システム。
- 内燃エンジンが、ガソリンまたはディーゼルエンジンである、請求項20に記載の排気ガス処理システム。
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US11187127B2 (en) * | 2019-06-28 | 2021-11-30 | Deere & Company | Exhaust gas treatment system and method with four-way catalyzed filter element |
BR112022011365A2 (pt) * | 2019-12-13 | 2022-08-23 | Basf Corp | Sistema de tratamento de emissão de redução de nox em uma corrente de exaustão de um motor de queima pobre e método para reduzir nox em uma corrente de exaustão de um motor de queima pobre |
US20230313719A1 (en) * | 2020-05-22 | 2023-10-05 | Briggs & Stratton, Llc | Small air-cooled engine with catalytic converter with ruthenium catalyst |
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