JP2006291918A - 排気ガス浄化触媒装置 - Google Patents
排気ガス浄化触媒装置 Download PDFInfo
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- 239000003054 catalyst Substances 0.000 claims abstract description 200
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 119
- 239000001301 oxygen Substances 0.000 claims abstract description 119
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 119
- 239000007789 gas Substances 0.000 claims abstract description 52
- 238000011144 upstream manufacturing Methods 0.000 claims abstract description 47
- 238000000746 purification Methods 0.000 claims abstract description 22
- 239000013078 crystal Substances 0.000 claims abstract description 19
- 229910052684 Cerium Inorganic materials 0.000 claims abstract description 16
- 229910052726 zirconium Inorganic materials 0.000 claims abstract description 16
- 239000011232 storage material Substances 0.000 claims description 53
- 229910052779 Neodymium Inorganic materials 0.000 claims description 5
- 239000000463 material Substances 0.000 abstract description 8
- 239000002131 composite material Substances 0.000 abstract 1
- 239000010948 rhodium Substances 0.000 description 32
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 25
- 239000000446 fuel Substances 0.000 description 17
- 230000000052 comparative effect Effects 0.000 description 15
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 9
- 230000008859 change Effects 0.000 description 7
- 239000011521 glass Substances 0.000 description 6
- 239000000203 mixture Substances 0.000 description 6
- 239000002002 slurry Substances 0.000 description 6
- 229910052751 metal Inorganic materials 0.000 description 5
- 239000002184 metal Substances 0.000 description 5
- 238000000034 method Methods 0.000 description 5
- 238000011068 loading method Methods 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 3
- 235000011114 ammonium hydroxide Nutrition 0.000 description 3
- 238000000975 co-precipitation Methods 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- 229910000510 noble metal Inorganic materials 0.000 description 3
- 229910052763 palladium Inorganic materials 0.000 description 3
- 229910052697 platinum Inorganic materials 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- 238000002360 preparation method Methods 0.000 description 3
- 230000004044 response Effects 0.000 description 3
- 238000005245 sintering Methods 0.000 description 3
- 230000004913 activation Effects 0.000 description 2
- 230000032683 aging Effects 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 229910002091 carbon monoxide Inorganic materials 0.000 description 2
- 210000002421 cell wall Anatomy 0.000 description 2
- HSJPMRKMPBAUAU-UHFFFAOYSA-N cerium(3+);trinitrate Chemical compound [Ce+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O HSJPMRKMPBAUAU-UHFFFAOYSA-N 0.000 description 2
- 238000010304 firing Methods 0.000 description 2
- 239000011259 mixed solution Substances 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 229920006395 saturated elastomer Polymers 0.000 description 2
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- 229910004625 Ce—Zr Inorganic materials 0.000 description 1
- 229910017493 Nd 2 O 3 Inorganic materials 0.000 description 1
- QGZKDVFQNNGYKY-UHFFFAOYSA-N ammonia Natural products N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 1
- 229910002056 binary alloy Inorganic materials 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- 230000003111 delayed effect Effects 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 238000001704 evaporation Methods 0.000 description 1
- 230000008020 evaporation Effects 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 238000005342 ion exchange Methods 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- 238000000691 measurement method Methods 0.000 description 1
- CFYGEIAZMVFFDE-UHFFFAOYSA-N neodymium(3+);trinitrate Chemical compound [Nd+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O CFYGEIAZMVFFDE-UHFFFAOYSA-N 0.000 description 1
- UJVRJBAUJYZFIX-UHFFFAOYSA-N nitric acid;oxozirconium Chemical compound [Zr]=O.O[N+]([O-])=O.O[N+]([O-])=O UJVRJBAUJYZFIX-UHFFFAOYSA-N 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000004043 responsiveness Effects 0.000 description 1
- 229910052703 rhodium Inorganic materials 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
- MWZNPHHDRLXXHO-UHFFFAOYSA-N rhodium;hydrate Chemical compound O.[Rh] MWZNPHHDRLXXHO-UHFFFAOYSA-N 0.000 description 1
- 239000000725 suspension Substances 0.000 description 1
- 230000036962 time dependent Effects 0.000 description 1
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Abstract
【解決手段】エンジンの排気通路に排気ガス流れの上流側と下流側とに配置されている2つの触媒3,4を備え、上流側触媒3及び下流側触媒4各々は酸素吸蔵材を含有し、上流側触媒3の酸素吸蔵材は、Ce及びZrを含有する複酸化物の結晶格子点又は格子点間にRhが配置されていて、下流側触媒4の酸素吸蔵材よりも同温度下における酸素吸蔵量がが多い。
【選択図】 図1
Description
上記上流側触媒及び下流側触媒各々は酸素吸蔵材を含有し、
上記上流側触媒の酸素吸蔵材は、Ce及びZrを含有する複酸化物の結晶格子点又は格子点間にRhが配置されていて、上記下流側触媒の酸素吸蔵材よりも同温度下における酸素吸蔵量が多いことを特徴とする。
上記下流側触媒の酸素吸蔵材は、上記上流側触媒の酸素吸蔵材とは成分が異なる複酸化物の結晶格子点又は格子点間にRhが配置されたものであり、
上記上流側触媒の酸素吸蔵材の方が上記下流側触媒の酸素吸蔵材よりも、同温度下における酸素吸蔵速度が大であることを特徴とする。
上記上流側触媒の酸素吸蔵材は、Ce、Zr及びNdの三元系複酸化物の結晶格子点又は格子点間にRhが配置されたものであり、
上記下流側触媒の酸素吸蔵材は、Ce及びZrの二元系複酸化物の結晶格子点又は格子点間にRhが配置されたものであることを特徴とする。
図1に示す触媒配置で実施例及び比較例の各触媒装置を構成するために、図2乃至図4に示す触媒A,B,Cの三種類を調製した。いずれもハニカム状担体(以下、単に担体という。)のセル壁5に、セル壁側に位置する内側触媒層6と、排気ガスに直接晒される外側触媒層7とを積層して形成したものである。
図2に示す触媒Aの内側触媒層6の触媒成分はPd/アルミナである。これは、Laを4質量%含有するγ−アルミナ粉末に触媒金属としてPdを後担持したものである。ここでいう「後担持」は、γ−アルミナ粉末等のサポート材に触媒金属溶液を接触させて焼成することによって触媒金属を担持したことを意味する。具体的には、蒸発乾固法を採用した。
Rh−CeZrNdOは、Ce、Zr、Nd及びRhの各溶液を原料として共沈法により調製した。その調製法を説明する。まず、オキシ硝酸ジルコニウム、硝酸第一セリウム、硝酸ネオジム(III)及び硝酸ロジウム各々の所定量と水とを混合して合計300mLとし、この混合溶液を室温で約1時間撹拌する。この混合溶液を80℃まで加熱昇温させた後、ガラス棒を用いて強く、素早く攪拌しつつ、別のビーカーに用意していた28%アンモニア水50mLを一気に加えて混合する。このアンモニア水の添加・混合は1秒以内に完了させる。アンモニア水の混合により白濁した溶液を一昼夜放置し、生成したケーキを遠心分離器にかけ、十分に水洗する。この水洗したケーキを約150℃の温度で乾燥させた後、400℃の温度に5時間保持し、次いで500℃の温度に2時間保持するという条件で焼成する。
内側触媒層6の形成にあたっては、Pd/アルミナとアルミナバインダとを各々担体に対して所定の担持量となるように秤量して混合し、これにイオン交換水を添加することによってスラリーを調製した。このスラリーに担体を浸漬して引き上げ、余分なスラリーを吹き飛ばす、という方法により、担体にスラリーをウォッシュコートした。次いで、これを150℃の温度で1時間乾燥し、540℃の温度で2時間焼成することによって内側触媒層6を形成した。
触媒Aの容量(担体容量)は0.9Lである。Pd/アルミナ及びPt/アルミナの担持量(担体1L当たりの担持量)は、γ−アルミナが50g/L、Pd及びPt各々が0.1g/Lとなるようにした。Rh−CeZrNdOの担持量は100g/Lとなるようにした。また、Rh−CeZrNdOにおけるCeZrNdO複酸化物の質量組成比は、CeO2:ZrO2:Nd2O3=22:68:10であり、該複酸化物におけるRh量は0.116質量%である。
図3に示す触媒Bでは、内側触媒層6の触媒成分は触媒Aと同じくPd/アルミナであるが、外側触媒層7の触媒成分はRh−CeZrOとPt/アルミナとの混合物であり、Rh−CeZrOを採用した点が触媒Aと異なる。このRh−CeZrOは、Ce及びZrの二元系複酸化物の結晶格子点又は格子点間にRhが配置されたものであり、触媒AのRh−CeZrNdOと同じく共沈法によって調製した。
図4に示す触媒Cは、内側触媒層6の触媒成分は触媒Aと同じくPd/アルミナであるが、外側触媒層7の触媒成分はRh/CeZrOとPt/アルミナとの混合物であり、Rh/CeZrOを採用した点が触媒Aと異なる。このRh/CeZrOは、Ce及びZrの二元系複酸化物にRhが後担持されたものである。
上記触媒A〜CのRh−CeZrNdO、Rh−CeZrO及びRh/CeZrOは、酸素吸蔵材として働く。そこで、これら酸素吸蔵材の酸素吸蔵量及び酸素吸蔵速度を調べた。その測定方法を説明する。
実施例1では、上流側触媒3として触媒Aを採用し、下流側触媒4として触媒Cを採用した。従って、上流側触媒3(触媒A)の酸素吸蔵材(Rh−CeZrNdO)は、下流側触媒4(触媒C)の酸素吸蔵材(Rh/CeZrO)よりも酸素吸蔵量が多く且つ酸素吸蔵速度も大ということになる。また、実施例1の上流側触媒3と下流側触媒4とを合わせた触媒容量は1.9Lである。
モデルガス流通反応装置及び排気ガス分析装置を用いて、上記実施例1,2及び比較例の各触媒装置のHC、CO及びNOxの浄化に関するライトオフ温度T50及び高温浄化率C400を測定した。実施例1,2及び比較例の各触媒A〜Cには大気雰囲気において1000℃で24時間保持するエージングを事前に施した。また、T50及びC400は、空燃比リッチのモデルガス(温度600℃)を10分間流した後に測定した。T50は、触媒に流入するモデルガス温度を常温から漸次上昇させていき、浄化率が50%に達したときの触媒入口のガス温度である。C400は触媒入口ガス温度が400℃のときの浄化率である。
2 排気通路
3 上流側触媒
4 下流側触媒
Claims (3)
- エンジンの排気通路に排気ガス流れの上流側と下流側とに配置されている2つの触媒を有する排気ガス浄化触媒装置であって、
上記上流側触媒及び下流側触媒各々は酸素吸蔵材を含有し、
上記上流側触媒の酸素吸蔵材は、Ce及びZrを含有する複酸化物の結晶格子点又は格子点間にRhが配置されていて、上記下流側触媒の酸素吸蔵材よりも同温度下における酸素吸蔵量が多いことを特徴とする排気ガス浄化触媒装置。 - 請求項1において、
上記下流側触媒の酸素吸蔵材は、上記上流側触媒の酸素吸蔵材とは成分が異なる複酸化物の結晶格子点又は格子点間にRhが配置されたものであり、
上記上流側触媒の酸素吸蔵材の方が上記下流側触媒の酸素吸蔵材よりも、同温度下における酸素吸蔵速度が大であることを特徴とする排気ガス浄化触媒装置。 - 請求項2において、
上記上流側触媒の酸素吸蔵材は、Ce、Zr及びNdの三元系複酸化物の結晶格子点又は格子点間にRhが配置されたものであり、
上記下流側触媒の酸素吸蔵材は、Ce及びZrの二元系複酸化物の結晶格子点又は格子点間にRhが配置されたものであることを特徴とする排気ガス浄化触媒装置。
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