JP6625537B2 - マンガン含有ディーゼル酸化触媒 - Google Patents
マンガン含有ディーゼル酸化触媒 Download PDFInfo
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- JP6625537B2 JP6625537B2 JP2016540477A JP2016540477A JP6625537B2 JP 6625537 B2 JP6625537 B2 JP 6625537B2 JP 2016540477 A JP2016540477 A JP 2016540477A JP 2016540477 A JP2016540477 A JP 2016540477A JP 6625537 B2 JP6625537 B2 JP 6625537B2
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- oxidation catalyst
- washcoat layer
- catalyst composite
- metal oxide
- coated
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- 239000003054 catalyst Substances 0.000 title claims description 219
- 238000007254 oxidation reaction Methods 0.000 title claims description 125
- 230000003647 oxidation Effects 0.000 title claims description 124
- 239000011572 manganese Substances 0.000 title claims description 104
- 229910052748 manganese Inorganic materials 0.000 title claims description 24
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 title claims description 19
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 125
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 92
- 239000000758 substrate Substances 0.000 claims description 91
- 239000002131 composite material Substances 0.000 claims description 83
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 60
- 239000010457 zeolite Substances 0.000 claims description 56
- 229910044991 metal oxide Inorganic materials 0.000 claims description 53
- 150000004706 metal oxides Chemical class 0.000 claims description 53
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 48
- 239000000463 material Substances 0.000 claims description 47
- 229910021536 Zeolite Inorganic materials 0.000 claims description 46
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 42
- 239000003870 refractory metal Substances 0.000 claims description 42
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- 238000000034 method Methods 0.000 claims description 23
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- UNYSKUBLZGJSLV-UHFFFAOYSA-L calcium;1,3,5,2,4,6$l^{2}-trioxadisilaluminane 2,4-dioxide;dihydroxide;hexahydrate Chemical compound O.O.O.O.O.O.[OH-].[OH-].[Ca+2].O=[Si]1O[Al]O[Si](=O)O1.O=[Si]1O[Al]O[Si](=O)O1 UNYSKUBLZGJSLV-UHFFFAOYSA-L 0.000 claims description 4
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- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 5
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- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 4
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Description
4NH3+4NO+O2→4N2+6H2O(標準SCR反応)(1)
4NH3+2NO+2NO2→4N2+6H2O(高速SCR反応)(2)
4NH3+3NO2→3.5N2+6H2O(遅いNO2−SCR反応)(3)
本明細書で使用する用語「担体」及び「基材」は、耐火性金属酸化物支持体が、典型的には、その上に触媒種を有する複数の支持体を含有するウォッシュコートの形態で配置されるモノリシック材料を指す。1以上の実施形態によると、この基材は、典型的には、DOC触媒を調製するために使用される材料のいずれかであり得、典型的には、金属又はセラミックハニカム構造体を含む。流路がそれを通る流体の流れに対して開いているように、基材の入口面又は出口面からそれを通って延びる微細な平行ガス流路を複数有する種類のモノリシック基材などの任意の適切な基材を用いてもよい。本質的に、流体入口から流体出口への直線路である流路は、その流路を通って流れるガスが触媒材料と接触するように、触媒材料が「ウォッシュコート」としてコーティングされる壁によって画定される。ウォッシュコートを、液体媒体中の支持体の指定された固形分(例えば、30〜50重量%)を含有するスラリーを調製することによって形成した後、担体基材上にコーティングして、乾燥させると、ウォッシュコート層が得られる。
1以上の実施形態による層状酸化触媒複合材料に有用な基材は、本質的に金属であってもよく、1以上の金属又は金属合金で構成されてもよい。金属基材は、波形シート又はモノリス形態など様々な形状で使用されてよい。適切な金属支持体は、チタン及びステンレス鋼などの耐熱性金属並びに金属合金だけでなく、鉄が実質成分又は主要成分である他の合金を含む。
1以上の実施形態による酸化触媒複合材料は、単層又は複数層で形成されてよい。場合により、触媒材料の1種類のスラリーを調製し、このスラリーを使用して、基材上に複数の層を形成することが適切であり得る。触媒複合材料は、公知の方法、例えば、初期湿潤により調製することができる。代表的な方法を以下に記載する。
トップウォッシュコート:トップウォッシュコートを以下のように調製した:5%アルミナ(Al2O3)Mnを含む支持体材料に、初期湿潤技術を用いてPt−アミン溶液を含浸させた。得られたPt含浸粉末を脱イオン水で希釈した。得られた水性スラリーのpHを、HNO3を用いてpH4.9に調整した。このスラリーを十分に混合し、次いで、1.5時間粉砕し、16μmの粒径を得た。ゼオライトをこのスラリーに添加し、このスラリーを十分に混合した。次いで、アルミナ結合剤を添加し、32%の固体を得た。このスラリーを、ボトムコートの上部のコーディエライト基材上にコーティングした。コーティングしたモノリスを乾燥させた後、2〜4時間、400〜550℃の範囲で焼成した。28.1g/ft3のPt添加量について、トップコート用のウォッシュコート添加量は約1.0g/in3であった。
トップウォッシュコート:トップウォッシュコートを以下のように調製した:アルミナ支持体材料に、初期湿潤技術を用いてPt−アミン溶液を含浸させた。得られたPt含浸粉末を脱イオン水で希釈した。得られた水性スラリーのpHを、HNO3の添加によってpH4.5に調整した。このスラリーを十分に混合し、次いで、粉砕し、18μmの粒径を得た。ゼオライトをこのスラリーに添加し、このスラリーを十分に混合した。次いで、アルミナ結合剤を添加し、33.3%の固体を得た。このスラリーを、ボトムコートの上部のコーディエライト基材上にコーティングした。コーティングしたモノリスを乾燥させた後、2〜4時間、400〜550℃の範囲で焼成した。28.1g/ft3のPt添加量について、トップコート用のウォッシュコート添加量は約1.0g/in3であった。
トップウォッシュコート:トップウォッシュコートを以下のように調製した:5%アルミナ(Al2O3)Mnを脱イオン水に添加した。得られた水性スラリーのpHを、HNO3の添加によってpH4.7に調整した。このスラリーを十分に混合し、次いで、粉砕し、19μmの粒径を得た。ゼオライトをこのスラリーに添加し、このスラリーを十分に混合した。次いで、アルミナ結合剤を添加し、34%の固体を得た。このスラリーを、ボトムコートの上部のコーディエライト基材上にコーティングした。コーティングしたモノリスを乾燥させた後、2〜4時間、400〜550℃の範囲で焼成した。0g/ft3のPt添加量について、トップコート用のウォッシュコート添加量は約1.0g/in3であった。
トップウォッシュコート:トップウォッシュコートを以下のように調製した:アルミナ支持体を脱イオン水に添加した。このスラリーを十分に混合し、次いで、粉砕し、22μmの粒径を得た。次いで、pHを、HNO3を用いてpH4.4に調整した。ゼオライトをこのスラリーに添加し、このスラリーを十分に混合した。次いで、アルミナ結合剤を添加し、33%の固体を得た。このスラリーを、ボトムコートの上部のコーディエライト基材上にコーティングした。コーティングしたモノリスを乾燥させた後、2〜4時間、400〜550℃の範囲で焼成した。0g/ft3のPt添加量について、トップコート用のウォッシュコート添加量は約1.0g/in3であった。
酸化触媒複合材料を、コージェライトハニカムモノリス基材上にPt含有及び/又はPd含有水性スラリーの2層をコーティングすることによって調製した。
酸化触媒複合材料を、コージェライトハニカムモノリス基材上にPt含有及び/又はPd含有水性スラリーの2層をコーティングすることによって調製した。
Claims (18)
- 希薄燃焼エンジンからの排ガス排出物の削減のための酸化触媒複合材料であって、
長さ、入口端及び出口端を有する担体基材と、前記担体上の酸化触媒の触媒材料を含み、前記酸化触媒の触媒材料が、第1の耐火性金属酸化物支持体、白金(Pt)成分及びパラジウム(Pd)成分を含み、そのPt:Pd比が10:1〜1:10の範囲にある第1のウォッシュコート層;並びに
第2の耐火性のMn含有金属酸化物支持体、ゼオライト、10g/ft 3 〜100g/ft 3 の範囲の量のPt成分、及び該Pt成分の10重量%以下であって、0.1g/ft 3 〜10g/ft 3 の範囲の量のPd成分を含む第2のウォッシュコート層
を含み、
希薄燃焼エンジン排ガス中の炭化水素及び一酸化炭素を削減し、かつNOをNO2に酸化するために使用され、
前記第1のウォッシュコート層が前記担体基材上にコーティングされ、前記第2のウォッシュコート層が前記第1のウォッシュコート層の上部にコーティングされる
酸化触媒複合材料。 - 希薄燃焼エンジンからの排ガス排出物の削減のための酸化触媒複合材料であって、
長さ、入口端及び出口端を有する担体基材と、前記担体上の酸化触媒の触媒材料を含み、前記酸化触媒の触媒材料が、第1の耐火性金属酸化物支持体、白金(Pt)成分及びパラジウム(Pd)成分を含み、そのPt:Pd比が10:1〜1:10の範囲にある第1のウォッシュコート層;並びに
第2の耐火性のMn含有金属酸化物支持体、ゼオライト、Pt成分を含む第2のウォッシュコート層
を含み、
希薄燃焼エンジン排ガス中の炭化水素及び一酸化炭素を削減し、かつNOをNO2に酸化するために使用され、
前記第1のウォッシュコート層が前記担体基材上にコーティングされ、前記第2のウォッシュコート層が前記第1のウォッシュコート層の上部にコーティングされ、
前記第2のウォッシュコート層がパラジウムを実質的に含まない、
酸化触媒複合材料。 - 前記第2の耐火性金属酸化物支持体のMn含有量が、0.1重量%〜30重量%の範囲にある、請求項1に記載の酸化触媒複合材料。
- 前記Mn含有量が、3〜10重量%の範囲にある、請求項3に記載の酸化触媒複合材料。
- 前記Mnが、前記耐火性金属酸化物支持体を有するMn含有固溶体、含浸によって前記耐火性金属酸化物支持体上に分散したMn表面、及び前記耐火性金属酸化物支持体粒子上の別々のマンガン酸化物粒子からなる群から選択される形態で存在する、請求項3に記載の酸化触媒複合材料。
- 前記Mnが、酢酸Mn、硝酸Mn、硫酸Mn、もしくはそれらの組み合わせから選択される可溶性Mn種、又はMnO、Mn2O3、MnO2、及びそれらの組み合わせから選択されるバルクMn酸化物由来である、請求項3に記載の酸化触媒複合材料。
- 前記第2の耐火性金属酸化物支持体が、アルミナ、シリカ、ジルコニア、チタニア、セリア、又はそれらの組み合わせを含む、請求項3に記載の酸化触媒複合材料。
- 前記第2のウォッシュコート層が、ZSM−5、ベータ、モルデナイト、Y型ゼオライト、菱沸石、フェリエライト、及びそれらの組み合わせからなる群から選択される6〜12員の環構造の形態で水熱安定ゼオライトを含む、請求項1に記載の酸化触媒複合材料。
- 前記第1の耐火性金属酸化物支持体が、アルミナ、シリカ、ジルコニア、チタニア、セリア、又はそれらの組み合わせを含む、請求項1に記載の酸化触媒複合材料。
- 前記第1のウォッシュコート層が、各成分を10g/ft3〜100g/ft3の範囲の量でPt成分及びPd成分を含む、請求項1に記載の酸化触媒複合材料。
- 前記第2のウォッシュコート層がバリウムを実質的に含まず、かつ前記第1のウォッシュコート層がゼオライトを実質的に含まない、請求項1に記載の酸化触媒複合材料。
- 前記Mnが、Fe、Ni、Co、Cu、Ce、Sn、Ir、In、又はそれらの組み合わせと共に添加される、請求項3に記載の酸化触媒複合材料。
- ディーゼルエンジンの排ガス流を処理する方法であって、請求項1〜12のいずれか一項に記載の酸化触媒複合材料と排ガス流を接触させることを含む方法。
- 前記酸化触媒複合材料のすぐ下流の、壁流フィルターモノリス上に配置されたSCR触媒組成物に前記排ガス流を通過させることをさらに含む、請求項13に記載の方法。
- 炭化水素、一酸化炭素、及び他の排ガス成分を含む希薄燃焼エンジンの排ガス流の処理システムであって、
排気マニホールドを介して前記希薄燃焼エンジンと流体連通する排気管;
前記担体基材がフロースルー基材である請求項1〜12のいずれか一項に記載の酸化触媒複合材料;並びに
前記酸化触媒複合材料の下流に位置する触媒すすフィルター及びSCR触媒;
を含むシステム。 - さらに希薄NOxトラップを含む、請求項15に記載のシステム。
- 前記希薄NOxトラップが、バリウム成分及びロジウム成分を含む、請求項16に記載のシステム。
- 前記SCR触媒が前記触媒すすフィルター上にコーティングされるか、あるいは
前記SCR触媒が、前記酸化触媒複合材料のすぐ下流のフロースルー基材上にコーティングされるとともに、前記触媒すすフィルターが前記SCR触媒の下流に存在する、請求項15に記載のシステム。
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KR102344639B1 (ko) | 2021-12-30 |
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KR20160098401A (ko) | 2016-08-18 |
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US20190262809A1 (en) | 2019-08-29 |
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RU2683771C1 (ru) | 2019-04-02 |
US20220234032A1 (en) | 2022-07-28 |
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