WO2010044453A1 - 排ガス浄化用触媒およびそれを用いた浄化方法 - Google Patents
排ガス浄化用触媒およびそれを用いた浄化方法 Download PDFInfo
- Publication number
- WO2010044453A1 WO2010044453A1 PCT/JP2009/067888 JP2009067888W WO2010044453A1 WO 2010044453 A1 WO2010044453 A1 WO 2010044453A1 JP 2009067888 W JP2009067888 W JP 2009067888W WO 2010044453 A1 WO2010044453 A1 WO 2010044453A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- exhaust gas
- catalyst
- magnesium oxide
- oxide
- noble metal
- Prior art date
Links
- 239000003054 catalyst Substances 0.000 title claims abstract description 196
- 238000000034 method Methods 0.000 title claims abstract description 57
- 238000000746 purification Methods 0.000 title claims description 41
- 239000011148 porous material Substances 0.000 claims abstract description 83
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims abstract description 71
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 claims abstract description 70
- 239000000395 magnesium oxide Substances 0.000 claims abstract description 69
- 229910052809 inorganic oxide Inorganic materials 0.000 claims abstract description 42
- 229910000510 noble metal Inorganic materials 0.000 claims abstract description 37
- 238000009826 distribution Methods 0.000 claims abstract description 23
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 claims abstract description 10
- 229910052753 mercury Inorganic materials 0.000 claims abstract description 10
- 239000002002 slurry Substances 0.000 claims description 31
- 150000003839 salts Chemical class 0.000 claims description 28
- 239000012736 aqueous medium Substances 0.000 claims description 14
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 13
- 238000001035 drying Methods 0.000 claims description 9
- 238000010304 firing Methods 0.000 claims description 9
- 239000010970 precious metal Substances 0.000 claims description 5
- 229910052761 rare earth metal Inorganic materials 0.000 claims description 5
- 229910052783 alkali metal Inorganic materials 0.000 claims description 3
- 150000001340 alkali metals Chemical class 0.000 claims description 3
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims description 3
- 150000001342 alkaline earth metals Chemical class 0.000 claims description 3
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims description 2
- 229910052748 manganese Inorganic materials 0.000 claims description 2
- 239000011572 manganese Substances 0.000 claims description 2
- 238000004519 manufacturing process Methods 0.000 claims description 2
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims description 2
- 229910052721 tungsten Inorganic materials 0.000 claims description 2
- 239000010937 tungsten Substances 0.000 claims description 2
- 238000001238 wet grinding Methods 0.000 claims 1
- 230000001590 oxidative effect Effects 0.000 abstract description 13
- 230000009970 fire resistant effect Effects 0.000 abstract 1
- 239000007789 gas Substances 0.000 description 99
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 89
- 235000012245 magnesium oxide Nutrition 0.000 description 59
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 27
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 19
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 15
- 229930195733 hydrocarbon Natural products 0.000 description 15
- 150000002430 hydrocarbons Chemical class 0.000 description 15
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 14
- 229910002091 carbon monoxide Inorganic materials 0.000 description 14
- 229910052697 platinum Inorganic materials 0.000 description 14
- 239000007864 aqueous solution Substances 0.000 description 11
- 230000000694 effects Effects 0.000 description 11
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 9
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 9
- 239000002245 particle Substances 0.000 description 9
- 239000010948 rhodium Substances 0.000 description 9
- -1 NOx Chemical class 0.000 description 8
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 8
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 8
- 239000012018 catalyst precursor Substances 0.000 description 8
- 229910052763 palladium Inorganic materials 0.000 description 8
- CHWRSCGUEQEHOH-UHFFFAOYSA-N potassium oxide Chemical compound [O-2].[K+].[K+] CHWRSCGUEQEHOH-UHFFFAOYSA-N 0.000 description 8
- 229910001950 potassium oxide Inorganic materials 0.000 description 8
- 229910052703 rhodium Inorganic materials 0.000 description 8
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 7
- 239000000203 mixture Substances 0.000 description 7
- 239000006185 dispersion Substances 0.000 description 6
- 238000005259 measurement Methods 0.000 description 6
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 6
- 239000000243 solution Substances 0.000 description 6
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 description 4
- 229910002651 NO3 Inorganic materials 0.000 description 4
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 4
- QVQLCTNNEUAWMS-UHFFFAOYSA-N barium oxide Chemical compound [Ba]=O QVQLCTNNEUAWMS-UHFFFAOYSA-N 0.000 description 4
- 238000002485 combustion reaction Methods 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 238000009792 diffusion process Methods 0.000 description 4
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 4
- 238000011156 evaluation Methods 0.000 description 4
- 150000004820 halides Chemical class 0.000 description 4
- YIXJRHPUWRPCBB-UHFFFAOYSA-N magnesium nitrate Chemical compound [Mg+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O YIXJRHPUWRPCBB-UHFFFAOYSA-N 0.000 description 4
- 239000004215 Carbon black (E152) Substances 0.000 description 3
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 3
- 229910021536 Zeolite Inorganic materials 0.000 description 3
- 239000003463 adsorbent Substances 0.000 description 3
- 150000004703 alkoxides Chemical class 0.000 description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 239000011324 bead Substances 0.000 description 3
- 229910052878 cordierite Inorganic materials 0.000 description 3
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 description 3
- 239000000446 fuel Substances 0.000 description 3
- 159000000003 magnesium salts Chemical class 0.000 description 3
- 150000002823 nitrates Chemical class 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 229910052760 oxygen Inorganic materials 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- 238000010298 pulverizing process Methods 0.000 description 3
- 239000004576 sand Substances 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- 238000001132 ultrasonic dispersion Methods 0.000 description 3
- 239000010457 zeolite Substances 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- IXSUHTFXKKBBJP-UHFFFAOYSA-L azanide;platinum(2+);dinitrite Chemical compound [NH2-].[NH2-].[Pt+2].[O-]N=O.[O-]N=O IXSUHTFXKKBBJP-UHFFFAOYSA-L 0.000 description 2
- 230000033228 biological regulation Effects 0.000 description 2
- 150000007942 carboxylates Chemical class 0.000 description 2
- 239000010419 fine particle Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 2
- 238000007654 immersion Methods 0.000 description 2
- 229910052741 iridium Inorganic materials 0.000 description 2
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 238000011056 performance test Methods 0.000 description 2
- SCVFZCLFOSHCOH-UHFFFAOYSA-M potassium acetate Chemical compound [K+].CC([O-])=O SCVFZCLFOSHCOH-UHFFFAOYSA-M 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 239000000377 silicon dioxide Substances 0.000 description 2
- 239000010935 stainless steel Substances 0.000 description 2
- 238000011144 upstream manufacturing Methods 0.000 description 2
- 229910000505 Al2TiO5 Inorganic materials 0.000 description 1
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- 229910052684 Cerium Inorganic materials 0.000 description 1
- 229910052692 Dysprosium Inorganic materials 0.000 description 1
- 229910052691 Erbium Inorganic materials 0.000 description 1
- 229910052693 Europium Inorganic materials 0.000 description 1
- 229910002060 Fe-Cr-Al alloy Inorganic materials 0.000 description 1
- 229910052688 Gadolinium Inorganic materials 0.000 description 1
- 229910052689 Holmium Inorganic materials 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- NIPNSKYNPDTRPC-UHFFFAOYSA-N N-[2-oxo-2-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 NIPNSKYNPDTRPC-UHFFFAOYSA-N 0.000 description 1
- 229910052779 Neodymium Inorganic materials 0.000 description 1
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 1
- 229910052777 Praseodymium Inorganic materials 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- 229910052772 Samarium Inorganic materials 0.000 description 1
- 229910052771 Terbium Inorganic materials 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 159000000021 acetate salts Chemical class 0.000 description 1
- 150000001242 acetic acid derivatives Chemical class 0.000 description 1
- 238000003916 acid precipitation Methods 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- 229910000272 alkali metal oxide Inorganic materials 0.000 description 1
- 229910000287 alkaline earth metal oxide Inorganic materials 0.000 description 1
- 229910000323 aluminium silicate Inorganic materials 0.000 description 1
- 229910052788 barium Inorganic materials 0.000 description 1
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910052792 caesium Inorganic materials 0.000 description 1
- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical compound [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 239000011575 calcium Substances 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 description 1
- 229910000420 cerium oxide Inorganic materials 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- HPXRVTGHNJAIIH-UHFFFAOYSA-N cyclohexanol Chemical compound OC1CCCCC1 HPXRVTGHNJAIIH-UHFFFAOYSA-N 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 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 1
- 238000002296 dynamic light scattering Methods 0.000 description 1
- KBQHZAAAGSGFKK-UHFFFAOYSA-N dysprosium atom Chemical compound [Dy] KBQHZAAAGSGFKK-UHFFFAOYSA-N 0.000 description 1
- UYAHIZSMUZPPFV-UHFFFAOYSA-N erbium Chemical compound [Er] UYAHIZSMUZPPFV-UHFFFAOYSA-N 0.000 description 1
- OGPBJKLSAFTDLK-UHFFFAOYSA-N europium atom Chemical compound [Eu] OGPBJKLSAFTDLK-UHFFFAOYSA-N 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
- UIWYJDYFSGRHKR-UHFFFAOYSA-N gadolinium atom Chemical compound [Gd] UIWYJDYFSGRHKR-UHFFFAOYSA-N 0.000 description 1
- KJZYNXUDTRRSPN-UHFFFAOYSA-N holmium atom Chemical compound [Ho] KJZYNXUDTRRSPN-UHFFFAOYSA-N 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 150000004679 hydroxides Chemical class 0.000 description 1
- 238000009434 installation Methods 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
- 238000007561 laser diffraction method Methods 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- UEGPKNKPLBYCNK-UHFFFAOYSA-L magnesium acetate Chemical compound [Mg+2].CC([O-])=O.CC([O-])=O UEGPKNKPLBYCNK-UHFFFAOYSA-L 0.000 description 1
- 235000011285 magnesium acetate Nutrition 0.000 description 1
- 239000011654 magnesium acetate Substances 0.000 description 1
- 229940069446 magnesium acetate Drugs 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
- ZADYMNAVLSWLEQ-UHFFFAOYSA-N magnesium;oxygen(2-);silicon(4+) Chemical compound [O-2].[O-2].[O-2].[Mg+2].[Si+4] ZADYMNAVLSWLEQ-UHFFFAOYSA-N 0.000 description 1
- 238000012423 maintenance Methods 0.000 description 1
- 229910052863 mullite Inorganic materials 0.000 description 1
- QEFYFXOXNSNQGX-UHFFFAOYSA-N neodymium atom Chemical compound [Nd] QEFYFXOXNSNQGX-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 1
- PIBWKRNGBLPSSY-UHFFFAOYSA-L palladium(II) chloride Chemical compound Cl[Pd]Cl PIBWKRNGBLPSSY-UHFFFAOYSA-L 0.000 description 1
- GPNDARIEYHPYAY-UHFFFAOYSA-N palladium(ii) nitrate Chemical compound [Pd+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O GPNDARIEYHPYAY-UHFFFAOYSA-N 0.000 description 1
- 230000035515 penetration Effects 0.000 description 1
- CLSUSRZJUQMOHH-UHFFFAOYSA-L platinum dichloride Chemical compound Cl[Pt]Cl CLSUSRZJUQMOHH-UHFFFAOYSA-L 0.000 description 1
- KGRJUMGAEQQVFK-UHFFFAOYSA-L platinum(2+);dibromide Chemical compound Br[Pt]Br KGRJUMGAEQQVFK-UHFFFAOYSA-L 0.000 description 1
- 238000002459 porosimetry Methods 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 239000011591 potassium Substances 0.000 description 1
- 235000011056 potassium acetate Nutrition 0.000 description 1
- PUDIUYLPXJFUGB-UHFFFAOYSA-N praseodymium atom Chemical compound [Pr] PUDIUYLPXJFUGB-UHFFFAOYSA-N 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
- 239000002994 raw material Substances 0.000 description 1
- 239000012495 reaction gas Substances 0.000 description 1
- VXNYVYJABGOSBX-UHFFFAOYSA-N rhodium(3+);trinitrate Chemical compound [Rh+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VXNYVYJABGOSBX-UHFFFAOYSA-N 0.000 description 1
- SONJTKJMTWTJCT-UHFFFAOYSA-K rhodium(iii) chloride Chemical compound [Cl-].[Cl-].[Cl-].[Rh+3] SONJTKJMTWTJCT-UHFFFAOYSA-K 0.000 description 1
- 229910052701 rubidium Inorganic materials 0.000 description 1
- IGLNJRXAVVLDKE-UHFFFAOYSA-N rubidium atom Chemical compound [Rb] IGLNJRXAVVLDKE-UHFFFAOYSA-N 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- KZUNJOHGWZRPMI-UHFFFAOYSA-N samarium atom Chemical compound [Sm] KZUNJOHGWZRPMI-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
- 229910052814 silicon oxide Inorganic materials 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- KKCBUQHMOMHUOY-UHFFFAOYSA-N sodium oxide Chemical compound [O-2].[Na+].[Na+] KKCBUQHMOMHUOY-UHFFFAOYSA-N 0.000 description 1
- 229910001948 sodium oxide Inorganic materials 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 229910001256 stainless steel alloy Inorganic materials 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 1
- 150000003467 sulfuric acid derivatives Chemical class 0.000 description 1
- GZCRRIHWUXGPOV-UHFFFAOYSA-N terbium atom Chemical compound [Tb] GZCRRIHWUXGPOV-UHFFFAOYSA-N 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- JUWGUJSXVOBPHP-UHFFFAOYSA-B titanium(4+);tetraphosphate Chemical compound [Ti+4].[Ti+4].[Ti+4].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O JUWGUJSXVOBPHP-UHFFFAOYSA-B 0.000 description 1
- 230000004580 weight loss Effects 0.000 description 1
- 238000004804 winding Methods 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
- 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
- B01J23/58—Platinum group metals with alkali- or alkaline earth metals
-
- 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
- F01N13/00—Exhaust or silencing apparatus characterised by constructional features ; Exhaust or silencing apparatus, or parts thereof, having pertinent characteristics not provided for in, or of interest apart from, groups F01N1/00 - F01N5/00, F01N9/00, F01N11/00
- F01N13/16—Selection of particular materials
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
- B01D53/9445—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC]
- B01D53/945—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC] characterised by a specific catalyst
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- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
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Definitions
- the present invention relates to an exhaust gas purification catalyst and an exhaust gas purification method using the catalyst. Specifically, the present invention aims to remove hydrocarbons (HC), carbon monoxide (CO), nitrogen oxides (NOx), particularly NOx, among harmful components contained in exhaust gas of gasoline engines and diesel engines.
- the present invention relates to an exhaust gas purifying catalyst and an exhaust gas purifying method using the catalyst.
- the above object is an exhaust gas purification catalyst in which a catalyst layer of a catalyst component containing a noble metal, magnesium oxide and a refractory inorganic oxide is formed on a three-dimensional structure, wherein the catalyst layer is intruded with mercury.
- This is achieved by an exhaust gas purifying catalyst characterized in that the distribution of voids between particles obtained by the method has two peaks due to magnesium oxide.
- a three-dimensional structure for example, a honeycomb carrier
- excess slurry is removed, and then dried and fired, moisture absorbed by the magnesium oxide evaporates during the drying and firing process, or magnesium.
- the oxide shrinks during the drying / calcination step, and pores having a large pore size (for example, 1 to 5 ⁇ m) can be formed in the catalyst layer. Therefore, when magnesium oxide is contained in the catalyst in this way, the pore volume of the catalyst layer increases, and the exhaust gas is easily diffused in the catalyst layer, and harmful substances such as HC, CO, NOx contained in the exhaust gas. It becomes possible to efficiently purify components, particularly NOx. Further, since the formed pores are based on the voids between the particles, even if the catalyst is exposed to a high temperature, it does not disappear due to so-called sintering or the like, and the purifying ability can be maintained for a long time.
- an exhaust gas purification catalyst using magnesium oxide as a catalyst component can achieve an excellent purification performance of CO, HC and NOx, particularly NOx, which are harmful components in the exhaust gas, and maintain the purification performance for a long period of time. can do.
- the ratio of the pore volume in the range of 1 to 5 ⁇ m corresponding to the first peak to the total pore volume or the first peak in the range of 0.1 to 1 ⁇ m corresponding to the second peak can be measured from the accumulated penetration amount in the range in the pore distribution measurement by the mercury intrusion method.
- the pore distribution of the catalyst layer containing magnesium oxide is measured, and in this pore distribution, the pore volume in the range of 1 to 5 ⁇ m corresponding to the first peak (P 1 ) and the total pore volume (P 2 ).
- P 1 and P 2 the ratio of the pore volume in the range corresponding to the first peak to the total pore volume is calculated by the following formula.
- ⁇ -alumina, etc. active alumina, titania, zirconia, single oxides such as silicon oxide (silica); complex oxides thereof such as alumina-titania, alumina-zirconia, titania-zirconia, zeolite, silica-alumina, etc. Is mentioned.
- single oxides such as ⁇ -alumina, silica, titania, zirconia, and composite oxides thereof are used.
- the above refractory inorganic oxides may be used alone or in the form of a mixture of two or more.
- the BET (Brunauer-Emmett-Teller) specific surface area of the refractory inorganic oxide is not particularly limited, but is preferably 20 to 750 m 2 / g, more preferably 50 to 350 m 2 / g.
- the average particle size of the refractory inorganic oxide powder is also not particularly limited, but is preferably 0.5 to 150 ⁇ m, more preferably 1 to 100 ⁇ m.
- the “average particle diameter” can be measured by an average value of particle diameters measured by a known method such as a laser diffraction method or a dynamic light scattering method.
- palladium in the case of palladium; halides such as palladium chloride; inorganic salts such as nitrate, sulfate, dinitrodiammine salt, tetraammine salt of palladium; carboxylates such as acetate; And hydroxide, alkoxide, oxide and the like.
- Preferred examples include nitrate, dinitrodiammine salt, tetraammine salt and acetate, and nitrate (palladium nitrate) is more preferred.
- the catalyst is dried at 100 to 250 ° C. for 10 minutes to 3 hours, and further calcined at 350 to 600 ° C. for 10 minutes to 5 hours, whereby the catalyst for exhaust gas purification of the present invention in which the catalyst component is supported on the three-dimensional structure. Can be manufactured.
- the catalyst precursor obtained as described above is charged and immersed in an aqueous solution obtained by dissolving a water-soluble noble metal salt in water, dried and fired to obtain a catalyst.
- the same method as described in the method (1) can be used for the step of dissolving the water-soluble noble metal salt in water to obtain an aqueous solution.
- the conditions for immersing the catalyst precursor in the aqueous solution are such that the noble metal in the aqueous solution is sufficiently uniformly mixed with the catalyst precursor and these noble metals are sufficiently supported on the catalyst precursor under the following drying and firing conditions. If there is no particular limitation.
- the catalyst precursor is immersed in an aqueous solution, dried at 100 to 250 ° C. for 10 minutes to 15 hours, and further calcined at 350 to 600 ° C. for 10 minutes to 5 hours, whereby the noble metal is supported on the catalyst precursor.
- the exhaust gas purification catalyst of the present invention can be manufactured.
- the above methods (1) and (2) are preferably used. More preferably, the above method (1) is used.
- Example 3 In Example 1, except that the amount of magnesium oxide used was changed from 3 g to 2.5 g and the amount of heat-resistant activated alumina was changed from 244 g to 244.5 g, a finished catalyst was prepared in the same manner as in Example 1. (C) was obtained. In this catalyst, 3 g / L of platinum, 2.5 g / L of magnesium oxide, 19 g / L of potassium oxide, and 244.5 g / L of alumina were supported on the support.
- Example 4 In Example 1, except that the amount of magnesium oxide used was changed from 3 g to 5 g and the amount of heat-resistant activated alumina was changed from 244 g to 242 g, the finished catalyst (D) was prepared in the same manner as in Example 1. Obtained. In this catalyst, platinum 3 g / L, magnesium oxide 5 g / L, potassium oxide 19 g / L, and alumina 242 g / L were supported on the support.
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Abstract
Description
細孔分布および細孔容積は、水銀圧入法により測定した。具体的には、200℃にて少なくとも30分間加熱処理(脱気)した担持触媒をサンプルとし、測定装置としてオートポアIII9420W(株式会社島津製作所製)を用い、0.5~60,000psia(0.0034~413.7MPa)の圧力範囲、等価時間10秒および60個の測定ポイントで測定し、細孔分布および細孔容積は、下記式(2)で表されるWashburnの式によって算出した。その際、水銀の表面張力は480N/mとし、水銀の接触角は130deg.とした。
協和化学工業製の酸化マグネシウム(商品名:キョーワマグ30)を3g、耐熱性活性γ-アルミナ(サソール製、商品名:SCFa140)を244g、酢酸カリウムを41g、白金を3g含むジニトロジアンミン白金水溶液および水を混合し、磁性ボールミルにより、常温で14時間、湿式粉砕して、水性スラリーを得た。この水性スラリーに、市販のコージェライト質モノリスハニカム担体(600セル/平方インチ、直径24mm、長さ66mm、体積0.030L)を浸漬し、余剰のスラリーを圧縮空気により吹き飛ばした。次に、150℃で水分減量がなくなるまで2時間乾燥し、さらに電気炉にて500℃で1時間焼成して、完成触媒(A)を得た。この触媒は、担体に対して、白金3g/L、酸化マグネシウム3g/L、酸化カリウム19g/L、およびアルミナ244g/Lが担持されていた。
実施例1において、協和化学工業製の酸化マグネシウム(商品名:キョーワマグ30)の代わりに、宇部マテリアルズ製の酸化マグネシウムUC95-Sを使う以外は、実施例1と同様の方法に従って、完成触媒(B)を得た。この触媒は、担体に対して、白金3g/L、酸化マグネシウム3g/L、酸化カリウム19g/L、およびアルミナ244g/Lが担持されていた。
実施例1において、酸化マグネシウムの使用量を3gから2.5gに変更し、耐熱性活性アルミナの使用量を244gから244.5gに変更する以外は、実施例1と同様の方法に従って、完成触媒(C)を得た。この触媒は、担体に対して、白金3g/L、酸化マグネシウム2.5g/L、酸化カリウム19g/L、およびアルミナ244.5g/Lが担持されていた。
実施例1において、酸化マグネシウムの使用量を3gから5gに変更し、耐熱性活性アルミナの使用量を244gから242gに変更する以外は、実施例1と同様の方法に従って、完成触媒(D)を得た。この触媒は、担体に対して、白金3g/L、酸化マグネシウム5g/L、酸化カリウム19g/L、およびアルミナ242g/Lが担持されていた。
実施例1において、酸化マグネシウムの使用量を3gから10gに変更し、耐熱性活性アルミナの使用量を244gから237gに変更する以外は、実施例1と同様の方法に従って、完成触媒(E)を得た。この触媒は、担体に対して、白金3g/L、酸化マグネシウム10g/L、酸化カリウム19g/L、およびアルミナ237g/Lが担持されていた。
実施例1において、酸化マグネシウムを加えない以外は、実施例1と同様の方法に従って、完成触媒(X)を得た。この触媒は、担体に対して、白金3g/L、酸化カリウム19g/L、およびアルミナ244g/Lが担持されていた。
実施例1~5で調製した完成触媒(A)~(E)、および比較例1で調製した完成触媒(X)について、下記試験を行なった。すなわち、まず触媒を電気炉にて800℃で50時間、耐久した。その後、ステンレス反応管に触媒を充填し、空間速度60,000h-1になるように下記表1に示される組成の反応ガスを導入し、触媒床入口300℃、350℃および400℃での平均NOx浄化率(%)を測定して、触媒性能を評価した。結果を下記表2および図1に示す。
上記実施例1および2で調製した完成触媒(A)および(B)、ならびに比較例1で調製した完成触媒(X)について、水銀圧入法を用いて触媒の細孔分布を測定した。上記それぞれの触媒について、第1および第2ピークの位置(μm)、前記第1ピークに相当する1~5μmの範囲の細孔容積の全細孔容積に対する比率(%)、ならびに前記第2ピークに相当する0.1~1μmの範囲の細孔容積の前記第1ピークに相当する1~5μmの範囲の細孔容積に対する比率を、下記表3に示す。また、完成触媒(A)、(B)および(X)のlog微分細孔容積分布のグラフを、図2に示す。
Claims (9)
- 三次元構造体に、貴金属、マグネシウム酸化物および耐火性無機酸化物を含む触媒成分の触媒層が形成されてなる排ガス浄化用触媒であって、
前記触媒層が、水銀圧入法で得られる細孔分布において、マグネシウム酸化物に起因するピークを2つ有することを特徴とする、排ガス浄化用触媒。 - 前期触媒層の細孔分布に存在する、前記マグネシウム酸化物に起因する2つのピークは、1~5μmの範囲に存在する第1ピークおよび0.1~1μmの範囲に存在する第2ピークである、請求項1に記載の排ガス浄化用触媒。
- 前記第1ピークに相当する1~5μmの範囲の細孔容積の、全細孔容積に対する割合が5~30%である、請求項2に記載の排ガス浄化用触媒。
- 前記第2ピークに相当する0.1~1μmの範囲の細孔容積の、前記第1ピークに相当する1~5μmの範囲の細孔容積に対する比率が0.5~30である、請求項3に記載の排ガス浄化用触媒。
- 前記マグネシウム酸化物の使用量が、三次元構造体1リットル当たり、0.5~10gである、請求項1~4のいずれか1項に記載の排ガス浄化用触媒。
- 触媒成分として、アルカリ金属、アルカリ土類金属、希土類元素、マンガンおよびタングステンからなる群より選択される少なくとも1種の元素の酸化物をさらに含む、請求項1~5のいずれか1項に記載の排ガス浄化用触媒。
- 前記マグネシウム酸化物は、酸化マグネシウムの形で触媒層に添加される、請求項1~6のいずれか1項に記載の排ガス浄化用触媒。
- 貴金属、マグネシウム酸化物および耐火性無機酸化物を水性媒体に分散し、湿式粉砕し、スラリーを得た後、三次元構造体を前記スラリー中に浸漬し、余剰のスラリーを除き、乾燥、焼成すること;または
水溶性貴金属塩を水に溶解し、耐火性無機酸化物に貴金属を担持して、貴金属担持耐火性無機酸化物を得、前記貴金属担持耐火性無機酸化物とマグネシウム酸化物を水性媒体に分散し、湿式粉砕して、スラリーを得た後、三次元構造体を前記スラリー中に浸漬し、余剰のスラリーを除き、乾燥、焼成すること、
を有する、請求項1~7のいずれか1項に記載の排ガス浄化用触媒の製造方法。 - 請求項1~7のいずれか1項に記載の排ガス浄化用触媒または請求項8に記載の方法にしたがって製造される排ガス浄化用触媒に対し、排ガスを接触させることを有する、排ガスの浄化方法。
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US13/124,147 US8722001B2 (en) | 2008-10-17 | 2009-10-16 | Catalyst for purification of exhaust gas and method for purification using the same |
CA2740565A CA2740565C (en) | 2008-10-17 | 2009-10-16 | Catalyst for purification of exhaust gas and method for purification using the same |
EP09820631.1A EP2343121B8 (en) | 2008-10-17 | 2009-10-16 | Exhaust gas purifying catalyst and purification method using same |
PL09820631T PL2343121T3 (pl) | 2008-10-17 | 2009-10-16 | Katalizator do oczyszczania gazu spalinowego i sposób oczyszczania przy jego użyciu |
CN200980141236.4A CN102186582B (zh) | 2008-10-17 | 2009-10-16 | 废气净化用催化剂以及使用该催化剂的净化方法 |
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WO2020137200A1 (ja) | 2018-12-28 | 2020-07-02 | ユミコア日本触媒株式会社 | 排気ガス浄化用触媒、その製造方法及びそれを用いた排気ガス浄化方法 |
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JP2017185465A (ja) * | 2016-04-07 | 2017-10-12 | トヨタ自動車株式会社 | 排ガス浄化触媒 |
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WO2020100831A1 (ja) | 2018-11-12 | 2020-05-22 | ユミコア日本触媒株式会社 | ガソリンエンジンの排気ガス浄化用触媒、その製造方法およびそれを用いた排気ガス浄化方法 |
JPWO2020100830A1 (ja) * | 2018-11-12 | 2021-10-14 | ユミコア日本触媒株式会社 | ディーゼルエンジンの排気ガス浄化用触媒、その製造方法およびそれを用いた排気ガス浄化方法 |
US11344864B2 (en) | 2018-11-12 | 2022-05-31 | Umicore Shokubai Japan Co., Ltd. | Diesel engine exhaust gas purification catalyst, production method therefor, and exhaust gas purification method using the same |
JP7241091B2 (ja) | 2018-11-12 | 2023-03-16 | ユミコア日本触媒株式会社 | ディーゼルエンジンの排気ガス浄化用触媒、その製造方法およびそれを用いた排気ガス浄化方法 |
US11813590B2 (en) | 2018-11-12 | 2023-11-14 | Umicore Shokubai Japan Co., Ltd. | Gasoline engine exhaust gas purification catalyst, production method therefor, and exhaust gas purification method using the same |
WO2020137200A1 (ja) | 2018-12-28 | 2020-07-02 | ユミコア日本触媒株式会社 | 排気ガス浄化用触媒、その製造方法及びそれを用いた排気ガス浄化方法 |
WO2021065238A1 (ja) * | 2019-10-01 | 2021-04-08 | 株式会社キャタラー | 排ガス浄化用触媒 |
JP7450359B2 (ja) | 2019-10-01 | 2024-03-15 | 株式会社キャタラー | 排ガス浄化用触媒 |
JP7425416B2 (ja) | 2021-01-08 | 2024-01-31 | 株式会社豊田中央研究所 | 触媒 |
Also Published As
Publication number | Publication date |
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CA2740565A1 (en) | 2010-04-22 |
EP2343121B1 (en) | 2022-01-12 |
KR101613997B1 (ko) | 2016-04-20 |
CN102186582B (zh) | 2015-05-13 |
JP5635410B2 (ja) | 2014-12-03 |
US8722001B2 (en) | 2014-05-13 |
CN102186582A (zh) | 2011-09-14 |
EP2343121A1 (en) | 2011-07-13 |
PL2343121T3 (pl) | 2022-02-21 |
EP2343121B8 (en) | 2022-02-16 |
JPWO2010044453A1 (ja) | 2012-03-15 |
CA2740565C (en) | 2016-10-25 |
EP2343121A4 (en) | 2012-10-24 |
KR20110074861A (ko) | 2011-07-04 |
US20110200506A1 (en) | 2011-08-18 |
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