JP6320918B2 - 低リンチャバサイト - Google Patents
低リンチャバサイト Download PDFInfo
- Publication number
- JP6320918B2 JP6320918B2 JP2014522995A JP2014522995A JP6320918B2 JP 6320918 B2 JP6320918 B2 JP 6320918B2 JP 2014522995 A JP2014522995 A JP 2014522995A JP 2014522995 A JP2014522995 A JP 2014522995A JP 6320918 B2 JP6320918 B2 JP 6320918B2
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- Prior art keywords
- molecular sieve
- phosphorus
- catalyst
- composition
- skeleton
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 102
- 239000002808 molecular sieve Substances 0.000 claims description 96
- 239000003054 catalyst Substances 0.000 claims description 71
- 229910052698 phosphorus Inorganic materials 0.000 claims description 65
- 239000011574 phosphorus Substances 0.000 claims description 62
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims description 61
- 239000000203 mixture Substances 0.000 claims description 42
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 40
- 239000000463 material Substances 0.000 claims description 37
- 238000000034 method Methods 0.000 claims description 33
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 30
- 239000013078 crystal Substances 0.000 claims description 30
- 239000010949 copper Substances 0.000 claims description 22
- 239000000758 substrate Substances 0.000 claims description 20
- 229910052782 aluminium Inorganic materials 0.000 claims description 19
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 18
- 239000000377 silicon dioxide Substances 0.000 claims description 18
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 16
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 16
- 229910052802 copper Inorganic materials 0.000 claims description 16
- 229910052710 silicon Inorganic materials 0.000 claims description 15
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 14
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 13
- 229910021529 ammonia Inorganic materials 0.000 claims description 13
- 239000010703 silicon Substances 0.000 claims description 12
- 229910004298 SiO 2 Inorganic materials 0.000 claims description 8
- 150000001875 compounds Chemical class 0.000 claims description 8
- 229910052742 iron Inorganic materials 0.000 claims description 7
- 150000002500 ions Chemical group 0.000 claims description 5
- 230000000737 periodic effect Effects 0.000 claims description 5
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 4
- 238000011144 upstream manufacturing Methods 0.000 claims description 4
- 229910018072 Al 2 O 3 Inorganic materials 0.000 claims description 3
- 239000004202 carbamide Substances 0.000 claims description 3
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 76
- 239000007789 gas Substances 0.000 description 46
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 29
- UNYSKUBLZGJSLV-UHFFFAOYSA-L calcium;1,3,5,2,4,6$l^{2}-trioxadisilaluminane 2,4-dioxide;dihydroxide;hexahydrate Chemical compound O.O.O.O.O.O.[OH-].[OH-].[Ca+2].O=[Si]1O[Al]O[Si](=O)O1.O=[Si]1O[Al]O[Si](=O)O1 UNYSKUBLZGJSLV-UHFFFAOYSA-L 0.000 description 29
- 229910052757 nitrogen Inorganic materials 0.000 description 21
- 229910052676 chabazite Inorganic materials 0.000 description 17
- 239000003638 chemical reducing agent Substances 0.000 description 17
- 238000003756 stirring Methods 0.000 description 16
- 125000004429 atom Chemical group 0.000 description 15
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 15
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 15
- 238000006243 chemical reaction Methods 0.000 description 14
- 238000002485 combustion reaction Methods 0.000 description 13
- 229910052751 metal Inorganic materials 0.000 description 13
- 239000002184 metal Substances 0.000 description 13
- 230000003647 oxidation Effects 0.000 description 13
- 238000007254 oxidation reaction Methods 0.000 description 13
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 12
- 230000015572 biosynthetic process Effects 0.000 description 12
- 229910052760 oxygen Inorganic materials 0.000 description 12
- 239000001301 oxygen Substances 0.000 description 11
- 229910017090 AlO 2 Inorganic materials 0.000 description 10
- 125000004437 phosphorous atom Chemical group 0.000 description 9
- 238000003786 synthesis reaction Methods 0.000 description 9
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 8
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 8
- 239000010953 base metal Substances 0.000 description 8
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 8
- 238000006722 reduction reaction Methods 0.000 description 7
- 229910000323 aluminium silicate Inorganic materials 0.000 description 6
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 6
- 230000003197 catalytic effect Effects 0.000 description 6
- 239000003153 chemical reaction reagent Substances 0.000 description 6
- 238000011065 in-situ storage Methods 0.000 description 6
- 238000004519 manufacturing process Methods 0.000 description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 6
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 5
- 229930195733 hydrocarbon Natural products 0.000 description 5
- 150000002430 hydrocarbons Chemical class 0.000 description 5
- 229910052697 platinum Inorganic materials 0.000 description 5
- 239000011148 porous material Substances 0.000 description 5
- 239000010457 zeolite Substances 0.000 description 5
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 4
- GQPLMRYTRLFLPF-UHFFFAOYSA-N Nitrous Oxide Chemical compound [O-][N+]#N GQPLMRYTRLFLPF-UHFFFAOYSA-N 0.000 description 4
- 229910021536 Zeolite Inorganic materials 0.000 description 4
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 4
- ANBBXQWFNXMHLD-UHFFFAOYSA-N aluminum;sodium;oxygen(2-) Chemical compound [O-2].[O-2].[Na+].[Al+3] ANBBXQWFNXMHLD-UHFFFAOYSA-N 0.000 description 4
- 229910002091 carbon monoxide Inorganic materials 0.000 description 4
- 239000000446 fuel Substances 0.000 description 4
- 229910021485 fumed silica Inorganic materials 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 4
- 229910052763 palladium Inorganic materials 0.000 description 4
- 235000011007 phosphoric acid Nutrition 0.000 description 4
- 229910001388 sodium aluminate Inorganic materials 0.000 description 4
- 229910001220 stainless steel Inorganic materials 0.000 description 4
- 239000010935 stainless steel Substances 0.000 description 4
- 229910052684 Cerium Inorganic materials 0.000 description 3
- 229910004283 SiO 4 Inorganic materials 0.000 description 3
- 239000002253 acid Substances 0.000 description 3
- 150000001768 cations Chemical class 0.000 description 3
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 description 3
- 239000011651 chromium Substances 0.000 description 3
- 239000002178 crystalline material Substances 0.000 description 3
- 239000003502 gasoline Substances 0.000 description 3
- 229910052738 indium Inorganic materials 0.000 description 3
- 238000005342 ion exchange Methods 0.000 description 3
- 239000011572 manganese Substances 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- 150000002739 metals Chemical class 0.000 description 3
- 230000001590 oxidative effect Effects 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- MGWGWNFMUOTEHG-UHFFFAOYSA-N 4-(3,5-dimethylphenyl)-1,3-thiazol-2-amine Chemical compound CC1=CC(C)=CC(C=2N=C(N)SC=2)=C1 MGWGWNFMUOTEHG-UHFFFAOYSA-N 0.000 description 2
- ATRRKUHOCOJYRX-UHFFFAOYSA-N Ammonium bicarbonate Chemical compound [NH4+].OC([O-])=O ATRRKUHOCOJYRX-UHFFFAOYSA-N 0.000 description 2
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 2
- OAKJQQAXSVQMHS-UHFFFAOYSA-N Hydrazine Chemical compound NN OAKJQQAXSVQMHS-UHFFFAOYSA-N 0.000 description 2
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 2
- 229910019142 PO4 Inorganic materials 0.000 description 2
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 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
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical group [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 0.000 description 2
- 239000001099 ammonium carbonate Substances 0.000 description 2
- 238000010531 catalytic reduction reaction Methods 0.000 description 2
- 238000005341 cation exchange Methods 0.000 description 2
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 2
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 2
- 229910052804 chromium Inorganic materials 0.000 description 2
- 239000003245 coal Substances 0.000 description 2
- 229910017052 cobalt Inorganic materials 0.000 description 2
- 239000010941 cobalt Substances 0.000 description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 2
- 239000008139 complexing agent Substances 0.000 description 2
- 230000002596 correlated effect Effects 0.000 description 2
- 239000002283 diesel fuel Substances 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 2
- 239000003949 liquefied natural gas Substances 0.000 description 2
- 239000003915 liquefied petroleum gas Substances 0.000 description 2
- 229910052748 manganese Inorganic materials 0.000 description 2
- 229910052759 nickel Inorganic materials 0.000 description 2
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 description 2
- 125000004430 oxygen atom Chemical group O* 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 2
- 239000010452 phosphate Substances 0.000 description 2
- 239000000376 reactant Substances 0.000 description 2
- 229910052703 rhodium Inorganic materials 0.000 description 2
- 239000010948 rhodium Substances 0.000 description 2
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 2
- 239000007858 starting material Substances 0.000 description 2
- 238000001308 synthesis method Methods 0.000 description 2
- 238000005287 template synthesis Methods 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 229910052718 tin Inorganic materials 0.000 description 2
- 239000011135 tin Substances 0.000 description 2
- 229910052719 titanium Inorganic materials 0.000 description 2
- 239000010936 titanium Substances 0.000 description 2
- 229910000013 Ammonium bicarbonate Inorganic materials 0.000 description 1
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 1
- -1 Platinum group metals Chemical class 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- 229910003902 SiCl 4 Inorganic materials 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- 229910006404 SnO 2 Inorganic materials 0.000 description 1
- 229910010413 TiO 2 Inorganic materials 0.000 description 1
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 1
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 1
- 238000010306 acid treatment Methods 0.000 description 1
- 235000012538 ammonium bicarbonate Nutrition 0.000 description 1
- BVCZEBOGSOYJJT-UHFFFAOYSA-N ammonium carbamate Chemical compound [NH4+].NC([O-])=O BVCZEBOGSOYJJT-UHFFFAOYSA-N 0.000 description 1
- 235000012501 ammonium carbonate Nutrition 0.000 description 1
- VZTDIZULWFCMLS-UHFFFAOYSA-N ammonium formate Chemical compound [NH4+].[O-]C=O VZTDIZULWFCMLS-UHFFFAOYSA-N 0.000 description 1
- 229910052787 antimony Inorganic materials 0.000 description 1
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 229910052797 bismuth Inorganic materials 0.000 description 1
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 description 1
- 229910052796 boron Inorganic materials 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- KXDHJXZQYSOELW-UHFFFAOYSA-N carbonic acid monoamide Natural products NC(O)=O KXDHJXZQYSOELW-UHFFFAOYSA-N 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 238000012993 chemical processing Methods 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 239000000571 coke Substances 0.000 description 1
- 230000002860 competitive effect Effects 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 230000001276 controlling effect Effects 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 230000000875 corresponding effect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 239000000295 fuel oil Substances 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 229910052732 germanium Inorganic materials 0.000 description 1
- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 description 1
- 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
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 238000005470 impregnation Methods 0.000 description 1
- 238000010348 incorporation Methods 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-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
- 239000011133 lead Substances 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 238000000386 microscopy Methods 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- 239000010955 niobium Substances 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 239000001272 nitrous oxide Substances 0.000 description 1
- 230000036961 partial effect Effects 0.000 description 1
- 239000013618 particulate matter Substances 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 239000006069 physical mixture Substances 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 238000007670 refining Methods 0.000 description 1
- 230000003252 repetitive effect Effects 0.000 description 1
- 229910052702 rhenium Inorganic materials 0.000 description 1
- WUAPFZMCVAUBPE-UHFFFAOYSA-N rhenium atom Chemical compound [Re] WUAPFZMCVAUBPE-UHFFFAOYSA-N 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 150000003384 small molecules Chemical class 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000004071 soot Substances 0.000 description 1
- 238000001694 spray drying Methods 0.000 description 1
- 230000003335 steric effect Effects 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 239000003440 toxic substance Substances 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
Images
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
- B01J29/72—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing iron group metals, noble metals or copper
- B01J29/76—Iron group metals or copper
- B01J29/763—CHA-type, e.g. Chabazite, LZ-218
-
- 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
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8621—Removing nitrogen compounds
- B01D53/8625—Nitrogen oxides
- B01D53/8628—Processes characterised by a specific catalyst
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
- B01D53/9404—Removing only nitrogen compounds
- B01D53/9409—Nitrogen oxides
- B01D53/9413—Processes characterised by a specific catalyst
- B01D53/9418—Processes characterised by a specific catalyst for removing nitrogen oxides by selective catalytic reduction [SCR] using a reducing agent in a lean exhaust gas
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
- B01J29/7015—CHA-type, e.g. Chabazite, LZ-218
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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Description
4NO+4NH3+3O2→4N2+6H2O
2NO2+4NH3+3O2→3N2+6H2O
NO+NO2+2NH3→2N2+3H2O
である。
(a)X2O3:(b)YO2:(c)(P2O5)
(式中、Xはアルミニウム、ホウ素、鉄、インジウム及び/又はガリウムなどの三価元素、好ましくはアルミニウムであり;Yはケイ素、スズ、チタン及び/又はゲルマニウムなどの四価元素、好ましくはケイ素であり;cは約0.005〜約0.050(0.05〜5モル%)、好ましくは約0.015〜約0.050(1.5〜5モル%)、より好ましくは約0.020〜約0.036(2〜3.6モル%)、更により好ましくは約0.026〜約0.030(2.6〜3モル%)又は約0.031〜約0.035(3.1〜3.5モル%)であり;a+b+c=1.00であり;b:aの比は少なくとも約5、好ましくは約5〜約40である)
を伴う組成物を有する。リンを有さないチャバサイトSSZ−13(米国特許第4544538号明細書)及び好ましくは25モル%よりはるかに高い最小リン含量を有するその類似体SAPO−34(米国特許第4440871号明細書)とは異なり、本発明の新規なモレキュラーシーブは、約0.5〜約5モル%のリン含量及び好ましくは少なくとも5のSARを有する。本発明のモレキュラーシーブは、その最も近いモレキュラーシーブ類似体と比べて独特に有益な物理的及び化学的特性を有するので、CHA骨格を有する新規な組成物を表す。
図1Aを参照すると、国際ゼオライト学会(IZA)により定義されるCHA骨格の単位格子が示されている。CHA骨格の各単位格子は36個の四面体サブユニットを有し、各サブユニットは好ましくはAl、Si及びPから個々に選択される中心T原子を有する。好ましくは、CHA結晶材料の個々の結晶は、1単位格子当たり約0.5〜約2.0個、より好ましくは1単位格子当たり約1.0〜約1.5個、更により好ましくは1単位格子当たり約1.1〜約1.3個の平均リン濃度を有する。骨格中のリン原子の位置は特に限定されない。すなわち、リン原子は、骨格中任意の位置に配置され得る。各単位格子は1個以上のリン原子を含有することができるが、本発明はそのように限定されない。あるいは、本発明は、個々の結晶の平均リン含量が上記範囲内にある限り、リン原子を有さない単位格子を有する結晶材料を含む。
本発明の低リンCHAモレキュラーシーブは、モレキュラーシーブ構造の形成中に(すなわち、インサイツで)合成することができる、又はモレキュラーシーブ構造を形成した後でモレキュラーシーブ構造に組み込むことができる(すなわち、ポストモレキュラーシーブ合成)。
本発明に使用するためのモレキュラーシーブ触媒は、ウォッシュコート、好ましくは例えば、ウォールフローフィルター又は焼結金属もしくはパーシャルフィルターを含む、金属もしくはセラミックフロースルーモノリス基材又はフィルタリング基材などの基材をコーティングするのに適したウォッシュコートの形態であり得る。したがって、本発明の別の態様は、本明細書に記載する触媒成分を含むウォッシュコートである。触媒成分に加えて、ウォッシュコート組成物は、アルミナ、シリカ、(非ゼオライト)シリカ−アルミナ、天然粘土、TiO2、CeO2、ZrO2、SnO2及びこれらの混合物からなる群から選択されるバインダーをさらに含み得る。
均質になるまで撹拌しながらフュームドシリカ75.80gを脱塩水500gと混ぜ合わせることにより、ゾル−ゲル反応組成物を調製した。アルミン酸ナトリウム約5.27〜5.89gをN,N,N−トリメチル−1−アダマンタモニウムヒドロキシド、TMADOH(25.5重量%)209.11gに溶解し、引き続いて水酸化ナトリウム6.75〜7.10gを溶解した。ベース溶液に、オルトリン酸(85重量%)0.364〜1.091gを均質化した。なお撹拌しながら、シリカ源をベース溶液に添加し、引き続いて脱塩水240gを添加し、混合物を均質になるまで撹拌させた。ステンレス鋼圧力反応器に装入する前にpHを測定した。最後に、撹拌しながら、ゾル−ゲルが以下のモル組成に達するまで脱塩水を反応器に添加した:
60SiO2:1.275≦x≦1.425Al2O3:0.075≦y≦0.225P2O5:6Na2O:12TMADOH:2640H2O
反応器を窒素でパージしたところ、混合物は170℃で3日後に結晶化した。
均質になるまで撹拌しながらフュームドシリカ75.80gを脱塩水500gと混ぜ合わせることにより、ゾル−ゲル反応組成物を調製した。アルミン酸ナトリウム約5.27gをN,N,N−トリメチル−1−アダマンタモニウムヒドロキシド、TMADOH(25.5重量%)209.11gに溶解し、引き続いて水酸化ナトリウム0.37〜7.10gを溶解した。ベース溶液に、オルトリン酸(85重量%)1.091gを均質化した。なお撹拌しながら、シリカ源をベース溶液に添加し、引き続いて脱塩水240gを添加し、混合物を均質になるまで撹拌させた。ステンレス鋼圧力反応器に装入する前にpHを測定した。最後に、撹拌しながら、ゾル−ゲルが以下のモル組成に達するまで脱塩水を反応器に添加した:
60SiO2:1.275Al2O3:0.225P2O5:2≦x≦6Na2O:12TMADOH:2640H2O
反応器を窒素でパージしたところ、混合物は170℃で3日後に結晶化した。
ゾル−ゲル反応組成物を2つの方法により調製した:
(a)均質になるまで撹拌しながらフュームドシリカ75.80gを脱塩水500gと混ぜ合わせた。アルミン酸ナトリウム5.27gをN,N,N−トリメチル−1−アダマンタモニウムヒドロキシド、TMADOH(25.5重量%)209.11gに溶解し、引き続いて水酸化ナトリウム7.10gを溶解した。ベース溶液に、オルトリン酸(85重量%)1.091gを均質化した。なお撹拌しながら、シリカ源をベース溶液に添加し、引き続いて脱塩水240gを添加し、混合物を均質になるまで撹拌させた。ステンレス鋼圧力反応器に装入する前にpHを測定した。最後に、撹拌しながら、ゾル−ゲルが以下のモル組成に達するまで脱塩水を反応器に添加した:
60SiO2:1.275Al2O3:0.225P2O5:6Na2O:12TMADOH:2640H2O
反応器を窒素でパージしたところ、混合物は170℃で3日後に結晶化した;
及び
(b)均質になるまで撹拌しながらフュームドシリカ75.80gを脱塩水500gと混ぜ合わせ、引き続いてオルトリン酸(85重量%)1.091gを添加した。アルミン酸ナトリウム5.27gをN,N,N−トリメチル−1−アダマンタモニウムヒドロキシド、TMADOH(25.5重量%)209.11gに溶解し、引き続いて水酸化ナトリウム7.10gを溶解した。なお撹拌しながら、シリカ源をベース溶液に添加し、引き続いて脱塩水240gを添加し、混合物を均質になるまで撹拌させた。ステンレス鋼圧力反応器に装入する前にpHを測定した。最後に、撹拌しながら、ゾル−ゲルが以下のモル組成に達するまで脱塩水を反応器に添加した:
60SiO2:1.275Al2O3:0.225P2O5:6Na2O:12TMADOH:2640H2O
反応器を窒素でパージしたところ、混合物は170℃で3日後に結晶化した。
以下の条件下で合成触媒活性試験(SCAT)リグを使用して新鮮な及び劣化した|Cu|[Al−Si−P−O]−CHA材料を試験した:500ppm NO、500ppm NH3、10%O2、10%H2O及び残りのN2:ならびに60000/時間の空間速度。比較のために、同様の試験を銅充填SSZ−13の試料に行った。
低リンCHAモレキュラーシーブの追加の合成を行い、約0.05モル%のリン、0.10モル%のリン、0.25モル%のリン、0.50モル%のリン、及び1.0モル%のリンを有する材料を製造する。
Claims (8)
- 結晶構造の少なくとも一部が、ケイ素、アルミニウム及びリンからなる群から選択される36個のT原子からなるチャバサイト骨格を有するモレキュラーシーブである結晶構造を含む組成物であって、
前記モレキュラーシーブが前記モレキュラーシーブ中の骨格ケイ素、アルミニウム及びリンの総モル基準で0.05〜5.0モル%の骨格リンを含み、
前記モレキュラーシーブが少なくとも10のシリカ対アルミナモル比を有する組成物。 - 前記モレキュラーシーブが無水モレキュラーシーブ基準で0.025〜5w/w%の銅及び/又は鉄をさらに含む、請求項1に記載の組成物。
- CHA骨格を有するモレキュラーシーブ材料を含む組成物であって、前記骨格はアルミニウム、ケイ素及びリンからなる群から選択される36個の連結T原子を有する周期的構築単位からなり、前記モレキュラーシーブ材料は骨格中の1周期的構築単位当たり0.5〜1.5個の原子の平均リン濃度を有し、少なくとも10のシリカ対アルミナモル比及び1より大きい骨格中のAl:Pモル比を有する、組成物。
- 前記モレキュラーシーブ材料がイオン交換された銅及び/又はイオン交換された鉄をさらに含む、請求項3に記載の組成物。
- i.CHA骨格と;
ii.0.5〜5.0モル%の骨格中のリンと;
iii.少なくとも10のシリカ対アルミナモル比のSiO2及びAl2O3と;
iv.少なくとも1の骨格中のアルミニウムとリンのモル比と;
v.無水モレキュラーシーブ基準で0.025〜5w/w%の銅及び/又は鉄と
を有するモレキュラーシーブ材料
を含む触媒活性ウォッシュコート。 - ウォールフローフィルター基材又はフロースルー基材上に請求項5に記載の触媒活性ウォッシュコートを含む触媒活性物品。
- 排気ガス中のNOx化合物のレベルを低下させるのに十分な時間及び温度で前記ガスを触媒と接触させるステップを含む、前記排気ガス中のNOxを還元する方法であって、前記触媒は請求項1に記載の組成物を含む触媒である方法。
- a.請求項6に記載の触媒活性物品と;
b.前記触媒物品の上流のアンモニア又は尿素源と
を含むエンジン排気ガス処理システム。
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GB2535274B (en) * | 2014-11-19 | 2019-06-12 | Johnson Matthey Plc | An exhaust system combining a molecular-sieve-containing SCR catalyst and a molecular-sieve-containing NOx adsorber catalyst |
GB201504986D0 (en) * | 2015-02-13 | 2015-05-06 | Johnson Matthey Plc | Oxidation catalyst for treating a natural gas emission |
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US11724249B2 (en) | 2018-10-23 | 2023-08-15 | N.E. Chemcat Corporation | Cu—P co-supported zeolite, and selective catalytic reduction catalyst and catalyst for exhaust gas using same |
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US9254481B2 (en) | 2016-02-09 |
US9878316B2 (en) | 2018-01-30 |
RU2014107473A (ru) | 2015-09-10 |
US20180147569A1 (en) | 2018-05-31 |
EP2736637B1 (en) | 2019-07-17 |
US20140193327A1 (en) | 2014-07-10 |
CN103764282A (zh) | 2014-04-30 |
JP2014528394A (ja) | 2014-10-27 |
EP2736637A2 (en) | 2014-06-04 |
BR112014001846A2 (pt) | 2017-02-21 |
US20160121317A1 (en) | 2016-05-05 |
RU2634702C2 (ru) | 2017-11-03 |
WO2013016522A2 (en) | 2013-01-31 |
CN108295893A (zh) | 2018-07-20 |
WO2013016522A3 (en) | 2013-06-13 |
US10258973B2 (en) | 2019-04-16 |
KR20140053240A (ko) | 2014-05-07 |
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