JP6775052B2 - 排ガス浄化用触媒 - Google Patents
排ガス浄化用触媒 Download PDFInfo
- Publication number
- JP6775052B2 JP6775052B2 JP2019061780A JP2019061780A JP6775052B2 JP 6775052 B2 JP6775052 B2 JP 6775052B2 JP 2019061780 A JP2019061780 A JP 2019061780A JP 2019061780 A JP2019061780 A JP 2019061780A JP 6775052 B2 JP6775052 B2 JP 6775052B2
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- Prior art keywords
- layer
- catalyst
- exhaust gas
- methane
- base material
- 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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- 239000003054 catalyst Substances 0.000 title claims description 234
- 238000000746 purification Methods 0.000 title claims description 95
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 237
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 210
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 186
- 239000007789 gas Substances 0.000 claims description 140
- 239000010948 rhodium Substances 0.000 claims description 113
- 239000000463 material Substances 0.000 claims description 85
- 238000002485 combustion reaction Methods 0.000 claims description 54
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims description 43
- 150000001342 alkaline earth metals Chemical class 0.000 claims description 43
- 229910052763 palladium Inorganic materials 0.000 claims description 33
- 229910052697 platinum Inorganic materials 0.000 claims description 27
- 238000005192 partition Methods 0.000 claims description 26
- 239000000446 fuel Substances 0.000 claims description 25
- 239000003345 natural gas Substances 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 9
- 239000002585 base Substances 0.000 description 77
- 239000002002 slurry Substances 0.000 description 66
- 229910052760 oxygen Inorganic materials 0.000 description 22
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 21
- 239000001301 oxygen Substances 0.000 description 21
- 229910000510 noble metal Inorganic materials 0.000 description 20
- 239000000843 powder Substances 0.000 description 18
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 17
- 239000011248 coating agent Substances 0.000 description 16
- 238000000576 coating method Methods 0.000 description 16
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 15
- 229910052751 metal Inorganic materials 0.000 description 15
- 239000002184 metal Substances 0.000 description 15
- 239000012298 atmosphere Substances 0.000 description 14
- 230000000694 effects Effects 0.000 description 14
- 229910052788 barium Inorganic materials 0.000 description 13
- 239000002131 composite material Substances 0.000 description 12
- 229930195733 hydrocarbon Natural products 0.000 description 12
- 150000002430 hydrocarbons Chemical class 0.000 description 12
- 239000002994 raw material Substances 0.000 description 11
- 229910052712 strontium Inorganic materials 0.000 description 11
- 238000005516 engineering process Methods 0.000 description 10
- 230000001603 reducing effect Effects 0.000 description 10
- 230000003197 catalytic effect Effects 0.000 description 9
- 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
- 230000001590 oxidative effect Effects 0.000 description 9
- 239000002245 particle Substances 0.000 description 9
- 238000012360 testing method Methods 0.000 description 9
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 8
- 229910002091 carbon monoxide Inorganic materials 0.000 description 8
- 238000002347 injection Methods 0.000 description 8
- 239000007924 injection Substances 0.000 description 8
- 238000000034 method Methods 0.000 description 8
- 238000007254 oxidation reaction Methods 0.000 description 8
- 231100000572 poisoning Toxicity 0.000 description 8
- 230000000607 poisoning effect Effects 0.000 description 8
- 238000011084 recovery Methods 0.000 description 8
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 7
- 238000011156 evaluation Methods 0.000 description 7
- 239000000203 mixture Substances 0.000 description 7
- 230000003647 oxidation Effects 0.000 description 7
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- 238000000629 steam reforming Methods 0.000 description 7
- 239000000956 alloy Substances 0.000 description 6
- 229910045601 alloy Inorganic materials 0.000 description 6
- 239000001257 hydrogen Substances 0.000 description 6
- 229910052739 hydrogen Inorganic materials 0.000 description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 6
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 5
- 239000007864 aqueous solution Substances 0.000 description 5
- 238000010304 firing Methods 0.000 description 5
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- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 4
- IWOUKMZUPDVPGQ-UHFFFAOYSA-N barium nitrate Chemical compound [Ba+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O IWOUKMZUPDVPGQ-UHFFFAOYSA-N 0.000 description 4
- 239000011575 calcium Substances 0.000 description 4
- 239000003381 stabilizer Substances 0.000 description 4
- DHEQXMRUPNDRPG-UHFFFAOYSA-N strontium nitrate Chemical compound [Sr+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O DHEQXMRUPNDRPG-UHFFFAOYSA-N 0.000 description 4
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 3
- 238000001035 drying Methods 0.000 description 3
- 239000003502 gasoline Substances 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- 238000003860 storage Methods 0.000 description 3
- 239000000758 substrate Substances 0.000 description 3
- 238000011144 upstream manufacturing Methods 0.000 description 3
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
- 238000004833 X-ray photoelectron spectroscopy Methods 0.000 description 2
- 230000002776 aggregation Effects 0.000 description 2
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- 239000011230 binding agent Substances 0.000 description 2
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- 238000006555 catalytic reaction Methods 0.000 description 2
- 239000003426 co-catalyst Substances 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 229910052878 cordierite Inorganic materials 0.000 description 2
- 239000013078 crystal Substances 0.000 description 2
- 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 2
- 239000002737 fuel gas Substances 0.000 description 2
- 239000010931 gold Substances 0.000 description 2
- 238000009434 installation Methods 0.000 description 2
- 229910052746 lanthanum Inorganic materials 0.000 description 2
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 2
- 230000005012 migration Effects 0.000 description 2
- 238000013508 migration Methods 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 2
- GPNDARIEYHPYAY-UHFFFAOYSA-N palladium(ii) nitrate Chemical compound [Pd+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O GPNDARIEYHPYAY-UHFFFAOYSA-N 0.000 description 2
- 239000012188 paraffin wax Substances 0.000 description 2
- NWAHZABTSDUXMJ-UHFFFAOYSA-N platinum(2+);dinitrate Chemical compound [Pt+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O NWAHZABTSDUXMJ-UHFFFAOYSA-N 0.000 description 2
- 229910052761 rare earth metal Inorganic materials 0.000 description 2
- 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 2
- 238000000638 solvent extraction Methods 0.000 description 2
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 2
- 229910052727 yttrium Inorganic materials 0.000 description 2
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 2
- 229910000505 Al2TiO5 Inorganic materials 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 1
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 1
- 229910002651 NO3 Inorganic materials 0.000 description 1
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 1
- 229910019142 PO4 Inorganic materials 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- 229910010413 TiO 2 Inorganic materials 0.000 description 1
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 1
- 150000001242 acetic acid derivatives Chemical class 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 239000003463 adsorbent Substances 0.000 description 1
- 230000002411 adverse Effects 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
- 238000005275 alloying Methods 0.000 description 1
- 230000033228 biological regulation Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000007664 blowing Methods 0.000 description 1
- 239000004202 carbamide Substances 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 150000001768 cations Chemical class 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 150000004696 coordination complex Chemical class 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 230000003111 delayed effect Effects 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000001747 exhibiting effect Effects 0.000 description 1
- 206010016766 flatulence Diseases 0.000 description 1
- 150000004675 formic acid derivatives Chemical class 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
- 150000004820 halides Chemical class 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 150000004679 hydroxides Chemical class 0.000 description 1
- 230000001771 impaired effect Effects 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 150000002500 ions Chemical class 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
- 238000003475 lamination Methods 0.000 description 1
- 238000007561 laser diffraction method Methods 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 150000002823 nitrates Chemical class 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
- 150000003891 oxalate salts Chemical class 0.000 description 1
- 239000008188 pellet Substances 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- 235000021317 phosphate Nutrition 0.000 description 1
- 150000003013 phosphoric acid derivatives Chemical class 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
- 229910052705 radium Inorganic materials 0.000 description 1
- HCWPIIXVSYCSAN-UHFFFAOYSA-N radium atom Chemical compound [Ra] HCWPIIXVSYCSAN-UHFFFAOYSA-N 0.000 description 1
- 229910001404 rare earth metal oxide Inorganic materials 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 238000000790 scattering method Methods 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
- 239000000377 silicon dioxide Substances 0.000 description 1
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- 229910052723 transition metal Inorganic materials 0.000 description 1
- 239000013585 weight reducing agent Substances 0.000 description 1
Images
Classifications
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- 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
- F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
- F01N3/24—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by constructional aspects of converting apparatus
- F01N3/28—Construction of catalytic reactors
- F01N3/2803—Construction of catalytic reactors characterised by structure, by material or by manufacturing of catalyst support
-
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- 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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- 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
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- 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
- B01D53/9472—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 zones
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- B01J23/002—Mixed oxides other than spinels, e.g. perovskite
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- 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
- B01J23/46—Ruthenium, rhodium, osmium or iridium
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Description
なお、白金族触媒は、酸化雰囲気に晒されると容易に酸素と結合し、触媒活性を失う。これを「酸素被毒」といい、例えばPd、Pt、およびRhは、酸化物(PdO、PtO、およびRhO)となって安定化される。被毒したPd、Pt、およびRhは、雰囲気が再び平衡ないしは還元雰囲気に戻る等して還元されることで、その活性が回復する。そのため、三元触媒は、主として、理論空燃比であるストイキ状態で燃焼する方式の内燃機関2の排ガスに対する浄化に用いられる。
PGMを単体で含む触媒層を備える触媒体を用いてメタン(CH4)の浄化を行うことで、各PGMを含む触媒層ごとのメタン浄化性能を確認した。
まず基材として、図2に示すような、オープンフロー(ストレートフロー)タイプのコージェライト製基材(外径120mm、全長115mm、嵩体積1.3L、セル数600cpsi(セル/in2))を用意した。
用意した各触媒体について、触媒評価装置を用い、天然ガス(CNG)車両の模擬排ガスにおけるメタン浄化率を調べた。この触媒評価装置は、マスフローコントローラ、加熱炉、O2センサー、エンジン排ガス分析計を備え、エンジン排ガスを模擬的に発生させるとともに、触媒体への流入ガスおよび触媒体からの流出ガスの成分を分析することができる。具体的には、以下の表1に示すガス成分を所定の割合で触媒評価装置にて混合し、CNG車両の排ガスを模擬的に発生させた。模擬排ガスは、表1に示すように酸素濃度を変化させることで、還元ガス成分に対する酸化ガス成分の割合(λ)をリッチ(0.9)からリーン(1.1)まで変化させた。なお、還元ガス成分に対する酸化ガス成分の割合は、λ=1がストイキであり、酸化ガスが還元ガスに対して等量であることを示す。上記ガスを500℃で触媒体に供給し、触媒体のメタン浄化率を測定した。メタン浄化率は、触媒体に流入する模擬排ガスのメタン濃度P1と、触媒体から流出する模擬排ガスのメタン濃度P2とを測定し、これらから次式:メタン浄化率(%)=[(P1−P2)/P1]×100;により算出した。その結果を図4に示した。
上記で用意した触媒体について、触媒体を酸素被毒させた状態で、メタンを原料とする水蒸気改質反応が生じ得るかどうかを調べた。具体的には、上記と同様の触媒評価装置を用い、先ずは、触媒体にF/C制御されたエンジンからの排ガスを模したリーン条件の排ガスを5分間供給し、触媒体を酸素被毒させた(条件1)。次いで、触媒体を水蒸気改質反応が生じ得る条件に5分間晒し、水蒸気反応が進行するかどうかを調べた(条件2)。触媒体への流入ガスの温度は300℃に固定し、リーン条件は、以下の表2の条件1に示す成分の排ガス(20%O2/N2)を触媒体に送るものとした。また、水蒸気改質条件は、表2の条件2に示す成分のガス(CH4+H2O/N2)を触媒体に送るものとした。これにより、触媒体から排出されるガス中の水素(H2)の濃度を測定し、その結果を図5に示した。
CH4 + H2O → CO +3H2 …(1)
CH4 +2H2O → CO2 +4H2 …(2)
CO + H2O → CO2 + H2 …(3)
触媒層としてのPd層、Pt層、Rh層の、触媒金属の使用量は同一としたまま、配置を異ならせた触媒体を用いてメタン(CH4)の浄化を行うことで、各触媒層の配置によるメタン浄化性能の違いを確認した。
まず基材として、オープンフロー(ストレートフロー)タイプのコージェライト製基材(外径120mm、全長115mm、嵩体積1.3L、セル数600cpsi(セル/in2))を用意した。
すなわち、基材のフロント側の端面から50%の長さ(0.5×Lw)までPdスラリーを供給したのち、過剰なスラリーをフロント側から所定の風速で吸引し、100℃で乾燥させたのち500℃で焼成することで、一層目のPd層を形成した。次いで、基材のリア側から50%の長さ(0.5×Lw)までPtスラリーを供給したのち、過剰なスラリーをリア側から所定の風速で吸引し、100℃で乾燥させたのち500℃で焼成することで、一層目のPtコート層を形成した。そして、基材のフロント側から80%の長さ(0.8×Lw)までRhスラリーを供給したのち、過剰なスラリーをフロント側から所定の風速で吸引し、100℃で乾燥させたのち500℃で焼成することで、二層目のRhコート層を形成した。これにより、例1の触媒体を得た。一層目のPd層とPt層とにおける基材の単位体積あたりの触媒の濃度は3g/Lとした。二層目のRhコート層における基材の単位体積あたりの触媒の濃度は0.15g/Lとした。また、基材の単位体積あたりの、Pd層のコート量は90g/L、Pt層のコート量は120g/L、Rh層のコート量は100g/Lとした。
一層目で基材のフロント側に供給するスラリーをPtスラリーに、リア側に供給するスラリーをPdスラリーに変え、その他は例1と同様にして、例2の触媒体を得た。
(例3)
一層目で基材のフロント側に供給するスラリーとリア側に供給するスラリーの両方をPdスラリーとし、その他は例1と同様にして、例3の触媒体を得た。
(例4)
一層目で基材のフロント側に供給するスラリーとリア側に供給するスラリーの両方をPtスラリーとし、その他は例1と同様にして、例4の触媒体を得た。
用意した各例の触媒体について、天然ガス(CNG)車両でメタンガスの浄化性能を評価した。具体的には、理論空燃比で燃焼する方式の筒内直接噴射天然ガスエンジン搭載車(ストイキCNG直噴車、1.5L)の排気経路に各例の触媒体をそれぞれ設置した。そして、この車両を、WLTC(Worldwide harmonized Light duty Test Cycle)で走行させたときの、メタン排出量(mg/km)を測定した。メタン排出量は、触媒体から排出された排ガス中のメタン濃度の測定結果から、次式:メタン排出量(mg/km)=排ガス中のメタン濃度(mg/L)×排ガス量(L)÷走行距離(km);に基づき算出した。その結果を、下記の表3と図6に示した。
触媒層としてのPd層、Pt層、Rh層の配置については一定にし、Pd層とPt層に、アルカリ土類金属成分であるバリウム(Ba)成分またはストロンチウム(Sr)成分を添加量を変化させて添加した触媒体を用いてメタン(CH4)の浄化を行うことで、メタン浄化性能の違いを確認した。基材は、参考例2と同じ、オープンフロー(ストレートハニカム)タイプのコージェライト製基材(外径120mm、全長115mm、嵩体積1.3L、セル数600cpsi(セル/in2))を用意した。
BaまたはSrを添加しないPt層については、参考例1、2と同様の原料を用い、Pt層のコート量が120g/Lとなるように層を形成したときに、Pt濃度が1.5g/Lとなるように、各Pt層原料の配合を調整してPtスラリーを調製した。すなわち、メタン排出量の変動をわかりやすくするために、メタン浄化能の高いPtの濃度は参考例と比較して控えめにした。
用意した各例の触媒体について、参考例2と同様に、天然ガス(CNG)車両でメタンガスの浄化性能を評価した。具体的には、理論空燃比で燃焼する方式の筒内直接噴射天然ガスエンジン搭載車(ストイキCNG直噴車、1.5L)の排気経路に各例の触媒体をそれぞれ設置した。そして、この車両を、WLTC(Worldwide harmonized Light duty Test Cycle)モードで走行させたときの、メタンの排出量(mg/km)を測定した。その結果を、下記の表4と、図7および図8に示した。表4中の「触媒層中濃度(%)」は、触媒層中のBaまたはSrの含有量(濃度、質量%)を算出した結果である。
2 内燃機関
5 触媒体
10 基材
12 セル
14 隔壁
20 触媒層
21 パラジウム(Pd)層
22 プラチナ(Pt)層
23 ロジウム(Rh)層
Claims (3)
- 内燃機関の排気経路に配置され、該内燃機関から排出される排ガスを浄化する排ガス浄化用触媒であって、
排ガスが流通するセルを区画する基材と、
前記基材の表面に設けられた触媒層と、
を備え、
前記触媒層は、
前記セルの排ガスが流入される側の端部である第1端部から排ガスが流出される側の端部である第2端部に向けて延設され、パラジウムを含むパラジウム層と、
前記第2端部から前記第1端部に向けて延設され、プラチナを含むプラチナ層と、
前記パラジウム層と前記プラチナ層の両方に積層され、ロジウムを含むロジウム層と、
を含み、
前記パラジウム層は、当該パラジウム層100gあたりにアルカリ土類金属を0.04モル以上0.16モル以下の含有量で含み、
前記プラチナ層は、アルカリ土類金属を実質的に含まない、排ガス浄化用触媒。 - 前記パラジウム層において、前記パラジウムに対する前記アルカリ土類金属のモル比は、1以上3以下である、請求項1に記載の排ガス浄化用触媒。
- 天然ガスを燃料とする内燃機関から排出される排ガスを浄化するために用いられる、請求項1または2に記載の排ガス浄化用触媒。
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