CN1386071A - 颗粒净化催化剂 - Google Patents
颗粒净化催化剂 Download PDFInfo
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- CN1386071A CN1386071A CN01802140A CN01802140A CN1386071A CN 1386071 A CN1386071 A CN 1386071A CN 01802140 A CN01802140 A CN 01802140A CN 01802140 A CN01802140 A CN 01802140A CN 1386071 A CN1386071 A CN 1386071A
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- catalyst
- alumina
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- 239000003054 catalyst Substances 0.000 title claims abstract description 118
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims abstract description 44
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims abstract description 44
- 230000003647 oxidation Effects 0.000 claims abstract description 43
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 43
- 238000000354 decomposition reaction Methods 0.000 claims abstract description 29
- 230000002378 acidificating effect Effects 0.000 claims abstract description 17
- 238000002485 combustion reaction Methods 0.000 claims abstract description 13
- 229910052697 platinum Inorganic materials 0.000 claims abstract description 11
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims abstract description 9
- CMPGARWFYBADJI-UHFFFAOYSA-L tungstic acid Chemical compound O[W](O)(=O)=O CMPGARWFYBADJI-UHFFFAOYSA-L 0.000 claims abstract description 7
- 229910052783 alkali metal Inorganic materials 0.000 claims abstract description 3
- 150000001340 alkali metals Chemical class 0.000 claims abstract description 3
- 229910052751 metal Inorganic materials 0.000 claims abstract description 3
- 239000002184 metal Substances 0.000 claims abstract description 3
- 150000003624 transition metals Chemical class 0.000 claims abstract description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 42
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 29
- 239000000203 mixture Substances 0.000 claims description 20
- 239000000377 silicon dioxide Substances 0.000 claims description 14
- 239000010948 rhodium Substances 0.000 claims description 11
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 8
- 229910021536 Zeolite Inorganic materials 0.000 claims description 8
- 239000010457 zeolite Substances 0.000 claims description 8
- 229910052703 rhodium Inorganic materials 0.000 claims description 5
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 claims description 4
- AQTIRDJOWSATJB-UHFFFAOYSA-K antimonic acid Chemical compound O[Sb](O)(O)=O AQTIRDJOWSATJB-UHFFFAOYSA-K 0.000 claims description 4
- 229910052593 corundum Inorganic materials 0.000 claims description 4
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 4
- 229910052737 gold Inorganic materials 0.000 claims description 4
- 239000010931 gold Substances 0.000 claims description 4
- 229910052741 iridium Inorganic materials 0.000 claims description 4
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 claims description 4
- 229910052763 palladium Inorganic materials 0.000 claims description 4
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims description 4
- 229910052707 ruthenium Inorganic materials 0.000 claims description 4
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 4
- 230000003197 catalytic effect Effects 0.000 claims description 2
- 229910052681 coesite Inorganic materials 0.000 claims description 2
- 229910052906 cristobalite Inorganic materials 0.000 claims description 2
- 229910052682 stishovite Inorganic materials 0.000 claims description 2
- 229910052905 tridymite Inorganic materials 0.000 claims description 2
- 150000002739 metals Chemical class 0.000 claims 1
- 239000013618 particulate matter Substances 0.000 abstract description 12
- 229910052784 alkaline earth metal Inorganic materials 0.000 abstract description 2
- 150000001342 alkaline earth metals Chemical class 0.000 abstract description 2
- 239000010970 precious metal Substances 0.000 abstract 2
- 238000010276 construction Methods 0.000 abstract 1
- 229910052723 transition metal Inorganic materials 0.000 abstract 1
- 239000000843 powder Substances 0.000 description 27
- 239000002245 particle Substances 0.000 description 24
- 230000000052 comparative effect Effects 0.000 description 19
- 239000007789 gas Substances 0.000 description 19
- 239000000758 substrate Substances 0.000 description 15
- 229910052760 oxygen Inorganic materials 0.000 description 12
- 239000007864 aqueous solution Substances 0.000 description 11
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 11
- 239000010410 layer Substances 0.000 description 11
- 239000001301 oxygen Substances 0.000 description 11
- 238000000034 method Methods 0.000 description 10
- 238000006243 chemical reaction Methods 0.000 description 9
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 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 7
- 239000000243 solution Substances 0.000 description 7
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 6
- 230000000694 effects Effects 0.000 description 5
- 230000001590 oxidative effect Effects 0.000 description 5
- 238000000746 purification Methods 0.000 description 5
- BNGXYYYYKUGPPF-UHFFFAOYSA-M (3-methylphenyl)methyl-triphenylphosphanium;chloride Chemical compound [Cl-].CC1=CC=CC(C[P+](C=2C=CC=CC=2)(C=2C=CC=CC=2)C=2C=CC=CC=2)=C1 BNGXYYYYKUGPPF-UHFFFAOYSA-M 0.000 description 4
- 239000011247 coating layer Substances 0.000 description 4
- 238000001556 precipitation Methods 0.000 description 4
- 239000002002 slurry Substances 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 3
- 238000001035 drying Methods 0.000 description 3
- 238000001704 evaporation Methods 0.000 description 3
- 239000000446 fuel Substances 0.000 description 3
- 229910017604 nitric acid Inorganic materials 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 3
- 230000009467 reduction Effects 0.000 description 3
- 230000002829 reductive effect Effects 0.000 description 3
- 238000011144 upstream manufacturing Methods 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical group [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- ITHZDDVSAWDQPZ-UHFFFAOYSA-L barium acetate Chemical compound [Ba+2].CC([O-])=O.CC([O-])=O ITHZDDVSAWDQPZ-UHFFFAOYSA-L 0.000 description 2
- 230000008020 evaporation Effects 0.000 description 2
- 238000005342 ion exchange Methods 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 239000002243 precursor Substances 0.000 description 2
- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Chemical compound [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 description 2
- 229910052814 silicon oxide Inorganic materials 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229910001928 zirconium oxide Inorganic materials 0.000 description 2
- IVORCBKUUYGUOL-UHFFFAOYSA-N 1-ethynyl-2,4-dimethoxybenzene Chemical compound COC1=CC=C(C#C)C(OC)=C1 IVORCBKUUYGUOL-UHFFFAOYSA-N 0.000 description 1
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 1
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-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
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 1
- SHPBBNULESVQRH-UHFFFAOYSA-N [O-2].[O-2].[Ti+4].[Zr+4] Chemical compound [O-2].[O-2].[Ti+4].[Zr+4] SHPBBNULESVQRH-UHFFFAOYSA-N 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 229910000287 alkaline earth metal oxide Inorganic materials 0.000 description 1
- 229910000379 antimony sulfate Inorganic materials 0.000 description 1
- MVMLTMBYNXHXFI-UHFFFAOYSA-H antimony(3+);trisulfate Chemical compound [Sb+3].[Sb+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O MVMLTMBYNXHXFI-UHFFFAOYSA-H 0.000 description 1
- 229910052788 barium Inorganic materials 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 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
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 229910052878 cordierite Inorganic materials 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 description 1
- 238000010494 dissociation reaction Methods 0.000 description 1
- 208000018459 dissociative disease Diseases 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 229910052742 iron Inorganic materials 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
- 230000007246 mechanism Effects 0.000 description 1
- 230000010534 mechanism of action Effects 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- 239000010955 niobium Substances 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- 230000002028 premature Effects 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
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- 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
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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
- B01D53/9404—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)
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- F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
- F01N3/021—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters
- F01N3/023—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles
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- F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
- F01N3/021—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters
- F01N3/033—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters in combination with other devices
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- F01N2370/02—Selection of materials for exhaust purification used in catalytic reactors
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- Environmental & Geological Engineering (AREA)
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- Exhaust Gas Treatment By Means Of Catalyst (AREA)
- Exhaust Gas After Treatment (AREA)
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Abstract
提供在比现有的更低的温度下容易燃烧捕集在柴油车的颗粒过滤器上的颗粒的颗粒净化催化剂。该颗粒催化剂的构成的特征在于,含有催化剂成分担持在酸性物质的第1担体上形成的NO氧化催化剂、以及催化剂成分担持在第2担体上形成的NO2分解催化剂而形成。优选NO氧化催化剂铂等贵金属担持在钨酸/氧化锆类酸性物质的第1担体上,NO2分解催化剂选自过渡金属的族的催化剂成分担持在氧化钛等的第2担体上,或者NO2分解催化剂选自碱金属和碱土金属的至少一种金属和铂等贵金属担持在氧化钛等第2担体上而形成。
Description
背景技术
本发明涉及一种用于燃烧除去柴油机等内燃机排出的废气中含有的烟灰状的颗粒(碳质微粒子)催化剂。
背景技术
从柴油机排出的废气含有颗粒物，是局部大气污染的主要原因之一。减少该颗粒物的排出量是环境问题中早期应解决的一个重要的课题。
为了减少该颗粒物的排除量，在柴油机的排气通路内配置颗粒过滤器，一旦捕集废气中的颗粒，就使捕集的颗粒着火燃烧，对该方式进行了研究。但是颗粒过滤器上捕集的颗粒不到大约600℃以上的高温不着火，与此相对，柴油机的废气的温度比600℃低得多，所以在废气流中燃烧除去颗粒需要降低颗粒的着火温度。
因此，现已知只要将催化剂担持在颗粒过滤器上，颗粒的着火温度就降低，例如特公平7-106290号公报中公开了使颗粒过滤器上担持铂族金属以及碱土类金属氧化物的混合物的颗粒过滤器，该颗粒过滤器在350℃～400℃比较低的低温下使颗粒着火，然后可以连续地使其燃烧。
但是柴油机的实际运转下废气的温度低于350℃的场合较多，在上述的约350℃～400℃的着火温度下不能完全地燃烧除去颗粒，通过过滤器的废气的压力损失大，产生燃费降低的障碍。而且，大量残存的颗粒一旦燃烧，使颗粒过滤器超过约800℃的温度，存在颗粒过滤器过早劣化的问题。
所以本发明的目的在于提供使颗粒过滤器上捕集的颗粒在比已有的更低的温度下容易氧化的颗粒净化催化剂。
发明内容
本发明的目的可以通过颗粒净化催化剂而实现，颗粒净化催化剂的特征在于：含有催化剂成分担持在酸性的第1担体上形成的NO氧化催化剂、以及催化剂成分担持在第2担体上形成的NO2分解催化剂而形成。
也就是，本发明为NO氧化催化剂和NO2分解催化剂共存的催化剂，具有NO氧化和NO2分解两个催化作用，促使颗粒氧化的催化剂。
本发明催化剂的作用机理考虑如下：
NO氧化催化剂加速如下反应。
NO2分解催化剂加速如下反应，放出活性氧(O*)。
该活性氧具有极高的氧化颗粒的活性。
这里活性氧也可以利用下述的O2解离反应产生。
O2→2O*
但是该3式的反应速度在低于300℃的温度下与所述(2)式的反应速度相比非常低。所以柴油机废气中的NO与O2相比，虽然浓度很小，加速所述(1)和(2)的反应可以有效地加速颗粒燃烧。
本发明的铂等催化剂成分担持在酸性担体上构成的NO氧化催化剂可以显著地加速所述(1)的反应。其原因在于催化剂成分在酸性担体上存在，也就是利用酸性担体的作用铂等催化剂成分经受酸性条件，所以氧化生成的酸性NO2可以容易地从催化剂成分脱离。
所以利用反应(1)大量的NO2来自NO氧化催化剂，然后NO2分解催化剂利用反应(2)由NO2生成活性氧，由此可以有效地从废气含有的NO供给多量的活性氧，即使低于大约300℃的废气温度，也可以高速地使颗粒氧化。
另外本发明对颗粒氧化机理进行如下考虑。颗粒的结构为微细的平面六角形的石墨结构聚集的结构，该顶端部分碳键合数减少，所以键的π电子密度比比平面部分高。为此，亲电性的活性氧O*被电子密度高的部分拉引，攻击碳键，从而氧化。也就是具有石墨结构的颗粒本质上容易受到亲电性的活性氧的氧化，所以大量地生成活性氧可以促进颗粒的低温氧化。
附图简要说明
图1(a)是担持本发明的催化剂的整体式过滤器壁剖面模式图。
图1(b)是担持本发明的催化剂的整体式过滤器剖面模式图。
图2(a)是显示担持本发明的催化剂状态的涂敷层内部的模式图。
图2(b)是显示担持本发明的催化剂状态的涂敷层内部的模式图。
发明的具体实施方案
构成本发明的颗粒净化催化剂之一的NO氧化催化剂是在酸性的担体上担持铂、金、钌、铑、铱、钯等具有NO氧化性能的催化剂成分而形成的。该酸性担体中例如有二氧化硅、二氧化硅-氧化铝、以及SiO2/Al2O3比为40以上的沸石类的均匀成分的粒子构成的粉末。
另外该酸性担体也可以是氧化锆或氧化铝类的弱酸性或两性粒子上通过包覆酸性物质的钨酸或锑酸等所担持的钨酸/氧化锆、锑酸/氧化铝等。这些例如可以通过使氧化锆或氧化铝浸渍在钨酸前体偏钨酸铵水溶液或锑酸前体硫酸锑水溶液中，使其蒸发干燥后烧结而得到。
然后可以利用蒸发干燥法、沉淀法、吸附法、离子交换法、还原析出法等使铂等催化剂成分担持在所述的酸性担体上。
构成本发明的另外一种颗粒净化催化剂的NO2分解催化剂是催化剂成分担持在第2担体上而形成的。该催化剂成分可以任意地选自过渡金属族，例如：铁、锰、钴、铜、镍、钒、钇、锌、铌、钼等。
这里使用碱金属或碱土金属作为NO2分解催化剂成分的场合，通过一并担持铂、金、钌、铑、铱、钯以及这些混合物组成的组中选择的贵金属，发现可以更进一步加速NO2分解。
担持NO2分解催化剂的催化剂成分的第2担体没有特别限定，可以选自氧化钛、氧化锆、氧化钛-氧化锆、氧化铝、氧化硅等弱酸性或两性的物质。
将NO2分解催化剂的催化成分担持在第2担体上时，和NO氧化催化剂同样，可以使用催化剂成分的溶液，利用蒸发干燥法、沉淀法、吸附法、离子交换法、还原析出法进行。
构成本发明的颗粒净化催化剂的成分的比例没有特别限定，重量比例为NO氧化催化剂/NO2分解催化剂的比为1/6～6/1、优选1/6～3/1。另外，在NO氧化催化剂中含有的催化剂成分优选酸性担体每100质量份为0.5～10质量份，更优选1.5～3质量份。另外，NO2分解催化剂中含有的催化剂成分优选第2担体每100质量份为1～40质量份，更优选2～10质量份。
所述的本发明的颗粒氧化催化剂担持在颗粒过滤器上，可以加速捕集在颗粒过滤器上的颗粒继续进行氧化。
该颗粒过滤器例如可以是堇青石制的整体式过滤器，图1显示使用本发明的催化剂的实施方式。
在该方式中，本发明的NO氧化催化剂和NO2分解催化剂作为包覆整体式过滤器的壁柱的涂敷层而存在。该涂敷层中如图2(a)所示，NO氧化催化剂和NO2分解催化剂可以无规状态混合存在，或者如图2(b)所示，也可以分别形成层的状态存在。实施例
NO氧化性能的担体的效果
作为担体使用钨酸/氧化锆(WO3/ZrO2)、二氧化硅、二氧化硅-氧化铝、MFI型沸石(SiO2/Al2O3＝40)、脱铝Y型沸石(SiO2/Al2O3＝200)、γ-氧化铝、氧化锆、Ba/γ-氧化铝，分别将各种担体涂敷在整体式基材上之后，用二亚硝化二氨合Pt溶液含浸担体，干燥·假烧结之后在650℃烧结1小时，得到在各种担体上每1升整体式基材担持2g Pt的催化剂。
这里WO3/ZrO2是利用如下所示的方法制成的NO氧化催化剂的担体。另外Ba/γ-氧化铝是利用比较例1的方法制成的担体。
这些催化剂中通入下述组成的气体，测定在200℃和250℃的气体温度下的NO→NO2的氧化率。结果示于表1。
气体组成：NO 250ppm+SO2 1ppm+H2O 5％+CO2 6％+O2 6％(其余：氮气)
表1：NO氧化性能的比较催化剂担体 NO氧化率(％)
200℃ 250℃WO3/ZrO2 64 93二氧化硅 45 92二氧化硅/氧化铝 34 92MFI沸石 66 92Y型沸石 62 93γ-氧化铝 15 90氧化锆 17 90Ba/γ-氧化铝 8.5 20催化剂成分：Pt 2g/1L整体式基材
由表1所示的结果比较酸性质担体的WO3/ZrO2、二氧化硅、二氧化硅-氧化铝、MFI型沸石、脱铝Y型沸石、γ-氧化铝(两性)、氧化锆(弱酸性)、Ba/γ-氧化铝(碱性)，可知200℃时NO氧化率明显高。这里Ba/γ-氧化铝的NO氧化率极低的原因考虑是碱性Ba影响Pt的氧化能力。
实施例1
在氢氧化锆粉末91质量份中添加20质量份的用WO3换算浓度为50质量％的偏钨酸铵水溶液，混合后在80℃下干燥过夜，然后在650℃烧结2小时，得到钨酸/氧化锆(WO3/ZrO2)粉末。
另外在γ-氧化铝粉末100质量份中添加85质量份的40质量％的醋酸钡水溶液，混合后在80℃下干燥过夜，然后在500℃烧结1小时，得到Ba/γ-氧化铝粉末。
在这些WO3/ZrO2粉末100质量份、Ba/γ-氧化铝粉末100质量份中，添加浓度40质量％的硝酸铝溶液60质量份、二氧化铈-氧化锆粉末40质量份、以及水200质量份，用球磨机混合8小时。
得到的浆料涂覆在整体式基材上，干燥后在650℃烧结1小时，在整体基材上形成含有WO3/ZrO2粉末和Ba/γ-氧化铝粉末的层。
然后在该层上含浸二亚硝化二氨络Pt水溶液，再含浸硝酸Rh水溶液，在500℃经过1小时烧结，得到每1升整体式基材上担持2g Pt和0.1g Rh的本发明的催化剂。
实施例2
和实施例1同样得到WO3/ZrO2粉末。
一方面相对100质量份的γ-氧化铝粉末，含浸5质量份的Fe，之后在80℃下干燥过夜，然后在500℃下烧结1小时，得到Fe/γ-氧化铝粉末。
在这些WO3/ZrO2粉末100质量份、Fe/γ-氧化铝粉末100质量份中，和实施例1同样添加硝酸铝溶液60质量份，二氧化铈-氧化锆粉末40质量份、以及200质量份水，利用球磨机混合8小时。
得到的浆料涂覆在整体式基材上，干燥后在650℃下烧结1小时，在整体基材上形成含有WO3/ZrO2粉末和Fe/γ-氧化铝粉末的层。
然后和实施例1同样含浸二亚硝化二氨络Pt水溶液和硝酸Rh水溶液，在500℃下烧结1小时，得到在1升整体式基材中担持2g Pt和0.1gRh的本发明的催化剂。
比较例1
在100质量份的γ-氧化铝粉末中，加入40质量％的醋酸钡水溶液85质量份，混合之后在80℃下干燥过夜，然后在500℃下烧结1小时，得到Ba/γ-氧化铝粉末。
在该Ba/γ-氧化铝粉末100质量份中添加浓度40质量％的硝酸铝溶液30质量份、二氧化铈-氧化锆粉末20质量份、以及水100质量份，利用球磨机混合8小时。
将得到的浆料涂覆在整体式基材上，干燥后在650℃下烧结1小时，形成含有Ba/γ-氧化铝粉末的层。
然后在该层中含浸二亚硝化二氨络Pt水溶液，再含浸硝酸Rh水溶液，在500℃下烧结1小时，得到在1升整体式基材中担持2g Pt和0.1gRh的比较例的催化剂。
比较例2
在100质量份的二氧化硅粉末中，加入40质量％的硝酸铝溶液30质量份，二氧化铈-氧化锆粉末20质量份、以及水100质量份，利用球磨机混合8小时。
将得到的浆料涂覆在整体式基材上，干燥后在650℃下烧结1小时，形成含有氧化硅粉末的层。
然后在该层中含浸二亚硝化二氨络Pt水溶液，再含浸硝酸Rh水溶液，在500℃下烧结1小时，得到在1升整体式基材中担持2g Pt和0.1gRh的比较例的催化剂。
另外，在该酸性担体氧化硅上担持Pt和Rh的催化剂用于比较试验，为在上游侧进行NO氧化生成NO2，在下游侧燃烧颗粒的方式。
-NO2分解性能的比较-
对于所述实施例1～23和比较例1～2的催化剂使用柴油机的废气测定NO2分解成NO的比例。运转条件设定为少(空燃比＝30)和多(空燃比＝14)分别在30秒期间和1秒的时间反复进行的条件，NO2分解率利用少条件下的下述废气组成测定。结果示于表2。这里比较例2的催化剂设置在该催化剂的下游堆积的颗粒的整体式过滤器(无催化剂)，在该整体式过滤器的出口测定NO2分解率。
气体组成：NO 250ppm+SO2 1ppm+H2O 5％+CO2 6％+O2 6％(其余：氮气)
表2 NO2分解性能的比较
催化剂 NO2分解率(％)
NO氧化催化剂 NO2分解催化剂 200℃ 250℃实施例1 Pt/WO3/ZrO2 Pt/Ba/γ-氧化铝 85 94实施例2 Pt/WO3/ZrO2 Fe/γ-氧化铝 88 90比较例1 Pt/Ba/γ-氧化铝 78 88比较例2 上游Pt/二氧化硅+整体式过滤器 2.1 3.5
催化剂成分：(Pt 2g+Rh 0.1g)/1L整体基体
由表2所示的结果可知，本发明的催化剂即使在低于300℃的温度，也显示非常高的NO2分解性能。一方面在γ-氧化铝担体上Pt和Ba共存的比较例中本发明的催化剂NO2分解性能有若干下降。另外比较例2的催化剂NO2分解性能几乎没有。其原因据认为是由于催化剂没有担持在整体式过滤器的结构的缘故。
-颗粒氧化速度的比较-
对于所述的实施例1～2和比较例1～2的催化剂使用柴油机的废气测定颗粒的氧化速度。运转条件设定为少(空燃比＝30)的连续条件，含有颗粒的下述的废气引入担持催化剂的颗粒过滤器中，利用过滤器的压力损失处于平衡的条件的颗粒供给速度求得颗粒的燃烧速度。结果示于表3。
气体组成：NO 250ppm+SO2 1ppm+H2O 5％+CO2 6％+O2 6％(其余：氮气)
表3 颗粒(PM)燃烧速度的比较
催化剂 PM燃烧速度(mg/sec/L)
NO氧化催化剂 NO2分解催化剂 200℃ 250℃实施例1 Pt/WO3/ZrO2 Pt/Ba/γ-氧化铝 0.04 0.12实施例2 Pt/WO3/ZrO2 Fe/γ-氧化铝 0.04 0.11比较例1 Pt/Ba/γ-氧化铝 0.012 0.05比较例2 上游Pt/二氧化硅+整体式过滤器 0.002 0.006催化剂成分：(Pt 2g+Rh 0.1g)/1L整体基体
由表3所示的结果可知，本发明的催化剂具有与比较例1的催化剂相比显著高的颗粒氧化速度，显然NO氧化催化剂和NO2分解催化剂共存的本发明的催化剂具有氧化颗粒的效果。另外比较例1的催化剂如表2所示虽然NO2分解性能高，但颗粒氧化速度相对于本发明的催化剂低。据认为这是因为表1所示的NO氧化能力是低温下的活性氧生成的一个原因，对于颗粒氧化具有重要的作用。
另外，比较例2显示极低的氧化速度，原因是即使只在上游侧供给NO2，由于NO2分解催化剂不存在，不放出活性氧，只利用NO2和颗粒的反应性，进行氧化。本发明中，NO的氧化和NO2的分解在催化剂内反复进行，由此低温下生成大量的活性氧，因而可以显著地提高颗粒的氧化速度。
工业实用性
如上所述，本发明具有可以在比已有的更低的温度下使柴油机排出的颗粒燃烧的效果。
Claims (4)
1.一种颗粒燃烧催化剂，其特征在于，催化剂成分是含有担持在酸性的第1担体上形成的NO氧化催化剂、以及催化剂成分担持在第2担体上形成的NO2分解催化剂而形成的。
2.如权利要求1所述的颗粒燃烧催化剂，其中，所述NO氧化催化剂是选自铂、金、钌、铑、铱、钯以及其混合物组成的族的催化成分，担持在选自二氧化硅、二氧化硅-氧化铝、SiO2/Al2O3比为40以上的沸石、钨酸/氧化锆、锑酸/氧化铝、及其混合物组成的组的酸性物质的第1担体上而形成的。
3.如权利要求1或2所述的颗粒燃烧催化剂，其中，所述NO2分解催化剂是选自过渡金属族的催化剂成分担持在选自氧化钛、氧化锆、氧化钛-氧化锆、氧化铝、二氧化硅及其混合物组成的组的第2担体上而形成的。
4.如权利要求1或2所述的颗粒燃烧催化剂，其中，所述NO2分解催化剂是选自碱金属和碱土金属的至少一种金属和铂、金、钌、铑、铱、钯以及其混合物组成的族的催化剂成分担持在选自氧化钛、氧化锆、氧化钛-氧化锆、氧化铝、氧化硅及其混合物组成的族的第2担体上而形成的。
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| US (1) | US7138353B2 (zh) |
| EP (1) | EP1224969B1 (zh) |
| JP (1) | JP4075292B2 (zh) |
| KR (1) | KR100495466B1 (zh) |
| CN (1) | CN1151873C (zh) |
| DE (1) | DE60138751D1 (zh) |
| ES (1) | ES2323758T3 (zh) |
| WO (1) | WO2002007879A1 (zh) |
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| CN102003251A (zh) * | 2009-09-02 | 2011-04-06 | 现代自动车株式会社 | 柴油机废气的后处理装置 |
| CN101600499B (zh) * | 2007-08-22 | 2013-02-13 | 三菱重工业株式会社 | 废气处理催化剂和废气处理系统 |
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| GB0308944D0 (en) * | 2003-04-17 | 2003-05-28 | Johnson Matthey Plc | Method of decomposing nitrogen dioxide |
| JP4508615B2 (ja) * | 2003-04-18 | 2010-07-21 | 三菱重工業株式会社 | 窒素酸化物の除去用触媒、触媒成型品、排ガス処理方法及び複合発電設備 |
| US7776784B2 (en) * | 2003-07-14 | 2010-08-17 | Nippon Oil Corporation | Hydrodesulfurization catalyst and hydrodesulfurization process for gasoline fractions |
| JP2007512133A (ja) * | 2003-11-24 | 2007-05-17 | ダウ グローバル テクノロジーズ インコーポレイティド | ディーゼル微粒子フィルター用触媒 |
| JP5144256B2 (ja) * | 2004-04-21 | 2013-02-13 | ダウ グローバル テクノロジーズ エルエルシー | 多孔質セラミック物体の強度の増大方法及びこの方法から製造された物体 |
| KR20070047322A (ko) * | 2004-07-26 | 2007-05-04 | 다우 글로벌 테크놀로지스 인크. | 개선된 촉매된 매연 필터 |
| GB0422549D0 (en) | 2004-10-12 | 2004-11-10 | Johnson Matthey Plc | Method of decomposing nitrogen dioxide |
| KR100681334B1 (ko) * | 2005-06-07 | 2007-02-09 | 희성엥겔하드주식회사 | 디젤산화 활성이 개선된 촉매조성물 |
| WO2007007889A1 (en) | 2005-07-12 | 2007-01-18 | Toyota Jidosha Kabushiki Kaisha | Exhaust gas purifying catalyst and process for producing it |
| KR101154925B1 (ko) | 2005-12-16 | 2012-06-13 | 에스케이이노베이션 주식회사 | 디젤차량의 입자제거필터용 촉매조성물 및 이를 이용한매연저감장치 |
| US7569511B2 (en) * | 2006-05-05 | 2009-08-04 | Basf Catalysts Llc | Catalyst composition for alcohol steam reforming |
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| EP2097154A2 (en) * | 2006-12-21 | 2009-09-09 | Dow Global Technologies Inc. | Improved soot filter |
| WO2009048994A2 (en) * | 2007-10-12 | 2009-04-16 | Dow Global Technologies Inc. | Improved thermal shock resistant soot filter |
| CA2701486A1 (en) * | 2007-12-21 | 2009-07-09 | Dow Global Technologies Inc. | Improved catalyzed soot filter and method (s) to make these |
| US8071504B2 (en) | 2008-12-19 | 2011-12-06 | Caterpillar Inc. | Exhaust system having a gold-platinum group metal catalyst |
| JP5293337B2 (ja) * | 2009-03-27 | 2013-09-18 | いすゞ自動車株式会社 | 内燃機関及び内燃機関の制御方法 |
| CN102482143A (zh) | 2009-09-30 | 2012-05-30 | 住友化学株式会社 | 玻璃料和利用其的碳微粒的氧化方法 |
| US20110120087A1 (en) * | 2009-11-23 | 2011-05-26 | Airflow Catalyst Systems | Apparatus with Catalyst for the Reduction of Nitrogen Dioxide (NO2) to Nitric Oxide (NO) by Chemical Means in a Diesel Catalytic Support |
| EP2682206A4 (en) | 2011-03-04 | 2014-09-17 | Toyota Motor Co Ltd | METAL PARTS, CATALYST FOR THE PURIFICATION OF PURIFICATION AND MANUFACTURING METHOD THEREFOR |
| JP5796630B2 (ja) * | 2011-08-23 | 2015-10-21 | トヨタ自動車株式会社 | 排ガス用浄化触媒およびその製造方法 |
| KR20150018877A (ko) | 2012-06-11 | 2015-02-24 | 레노비아 인코포레이티드 | 1,6-헥산디올로부터 아디프산의 제조방법 |
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| JP6044605B2 (ja) * | 2014-08-25 | 2016-12-14 | マツダ株式会社 | 触媒付パティキュレートフィルタ及びその製造方法 |
| US10105627B2 (en) | 2014-08-25 | 2018-10-23 | Mazda Motor Corporation | Particulate filter provided with catalyst and method for manufacturing said filter |
| CN109806882A (zh) * | 2019-03-18 | 2019-05-28 | 山东大业联合新能源设备有限公司 | 一种sco脱硝新能源复合材料 |
| CN110732326A (zh) * | 2019-10-16 | 2020-01-31 | 湖北航特装备制造股份有限公司 | 一种柴油机颗粒物捕集器用催化剂及其制备方法 |
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-
2000
- 2000-07-24 JP JP2000227577A patent/JP4075292B2/ja not_active Expired - Fee Related
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2001
- 2001-07-23 US US10/088,648 patent/US7138353B2/en not_active Expired - Fee Related
- 2001-07-23 DE DE60138751T patent/DE60138751D1/de not_active Expired - Lifetime
- 2001-07-23 KR KR10-2002-7003773A patent/KR100495466B1/ko not_active IP Right Cessation
- 2001-07-23 EP EP01950040A patent/EP1224969B1/en not_active Expired - Lifetime
- 2001-07-23 ES ES01950040T patent/ES2323758T3/es not_active Expired - Lifetime
- 2001-07-23 WO PCT/JP2001/006351 patent/WO2002007879A1/ja active IP Right Grant
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101600499B (zh) * | 2007-08-22 | 2013-02-13 | 三菱重工业株式会社 | 废气处理催化剂和废气处理系统 |
| CN102003251A (zh) * | 2009-09-02 | 2011-04-06 | 现代自动车株式会社 | 柴油机废气的后处理装置 |
| CN102003251B (zh) * | 2009-09-02 | 2017-04-12 | 现代自动车株式会社 | 柴油机废气的后处理装置 |
Also Published As
| Publication number | Publication date |
|---|---|
| WO2002007879A1 (fr) | 2002-01-31 |
| US20020197191A1 (en) | 2002-12-26 |
| CN1151873C (zh) | 2004-06-02 |
| KR100495466B1 (ko) | 2005-06-16 |
| EP1224969B1 (en) | 2009-05-20 |
| EP1224969A1 (en) | 2002-07-24 |
| JP2002035587A (ja) | 2002-02-05 |
| KR20020033820A (ko) | 2002-05-07 |
| JP4075292B2 (ja) | 2008-04-16 |
| ES2323758T3 (es) | 2009-07-24 |
| EP1224969A4 (en) | 2003-09-03 |
| DE60138751D1 (de) | 2009-07-02 |
| US7138353B2 (en) | 2006-11-21 |
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