JP2017214928A - 酸化触媒を含む希薄燃焼内燃機関の排気ガス処理装置及び酸化触媒の酸化活性の回復方法 - Google Patents
酸化触媒を含む希薄燃焼内燃機関の排気ガス処理装置及び酸化触媒の酸化活性の回復方法 Download PDFInfo
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- JP2017214928A JP2017214928A JP2017128907A JP2017128907A JP2017214928A JP 2017214928 A JP2017214928 A JP 2017214928A JP 2017128907 A JP2017128907 A JP 2017128907A JP 2017128907 A JP2017128907 A JP 2017128907A JP 2017214928 A JP2017214928 A JP 2017214928A
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- oxidation catalyst
- exhaust gas
- catalyst
- monolith substrate
- oxidation
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Links
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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
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- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J38/00—Regeneration or reactivation of catalysts, in general
- B01J38/04—Gas or vapour treating; Treating by using liquids vaporisable upon contacting spent catalyst
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- B01D—SEPARATION
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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
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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
- F01N3/0807—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by using absorbents or adsorbents
- F01N3/0814—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by using absorbents or adsorbents combined with catalytic converters, e.g. NOx absorption/storage reduction catalysts
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- 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
- B01D53/944—Simultaneously removing carbon monoxide, hydrocarbons or carbon making use of oxidation catalysts
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- 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
- B01D53/96—Regeneration, reactivation or recycling of reactants
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- 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
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
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- 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
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Abstract
【解決手段】希薄燃焼内燃機関と、エンジン管理手段と、エンジンの排気ガスを処理するための排気系とを備えており、前記排気系が、第1のハニカムモノリス基材に配置された第1の酸化触媒を備え、前記第1の酸化触媒は、少なくとも1つの還元可能な酸化物を含む第1の金属酸化物支持体上に支持された白金を含んでおり、前記第1の酸化触媒が、アルカリ金属およびアルカリ土類金属を実質的に含まず、前記エンジン管理手段が、使用時に、前記第1の酸化触媒に進入する排気ガスのラムダ組成を濃いラムダ組成へと間欠的に調節する。
【選択図】図3
Description
NO+1/2O2→NO2(1)、および
BaO+NO2+1/2O2→Ba(NO3)2(2)
であり、反応(2)において、白金上の活発な酸化部位において酸化チッ素が酸素と反応し、NO2が形成される。反応(3)が、無機硝酸塩の形態での貯蔵物質によるNO2の吸着を含んでいる。
Ba(NO3)2→BaO+2NO+3/2O2またはBa(NO3)2→BaO+2NO2+1/2O2(3)、ならびに
NO+CO→1/2N2+CO2(4)
(他の反応として、Ba(NO3)2+8H2→BaO+2NH3+5H2O、およびそれに続くNH3+NOx→N2+yH2Oまたは2NH3+2O2+CO→N2+3H2O+CO2、などが挙げられる)。
(1)PGMをセリアなどの第1の金属酸化物支持体上に支持することによって、PGMの焼結の程度を大幅に軽減することができ、したがって熱的な経年劣化の後でも多数の触媒活性部位が残る。しかしながら、各々の触媒部位は、PtまたはPtPd触媒部位の酸化物の特性ゆえに、きわめて活発というわけではない。PGMの最も活発な形態は、その金属状態であり、我々は、きわめて驚くべきことに、本発明による触媒に関して、濃い条件に曝されたときに活発な状態が実質的に再生されることを発見した。
(2)セリアおよびセリア−ジルコニアが、NOxトラップにおいて、NOx貯蔵機能を改善するために、K、Cs、Ba、Srなどの他の金属との組み合わせにて使用されている。しかしながら、本発明においては、そのような追加の金属は、HCおよびCOの酸化を妨げる効果があるがゆえに、好ましくは使用されない。
(3)従来の層が、計画時の濃い事象を実行することができない場合に容認できる触媒活性を維持するために使用される。例えば、比較的高い希薄温度に長時間にわたって曝された後には、酸化活性の大部分が、層のうちの少なくとも1つにおいて生じる。
1平方インチ当たり400セルのハニカム貫流コーディエライトモノリス基材を、2層の従来の触媒でコートした。第1の層を、1.67gin−3のAl2O3および0.33gin−3のベータゼオライト(この下側層について、合計2gin−3のウォッシュコート量)ならびにPtPdで構成し、第2の上側層を、0.833gin−3のAl2O3および0.167gin−3のベータゼオライト(この上側層について、合計1gin−3のウォッシュコート量)ならびにPtのみで構成した。この第1の層を、国際公開第99/47260号に開示の方法、すなわち(a)基材モノリスの上側の第1の端部に閉じ込め手段を配置するステップと、(b)所定の量の第1のウォッシュコートコーティング成分を前記閉じ込め手段へと与えるステップと、(c)圧力または真空を加えることによって、前記第1のウォッシュコートコーティング成分を基材モノリスの少なくとも一部分へと引き込み、前記量の実質的にすべてを基材モノリス内に保持するステップとを含む方法(ステップ(a)の次にステップ(b)の順序でも、ステップ(b)の次にステップ(a)の順序でもよい)を使用して、PtおよびPdの塩を含むウォッシュコートとして未使用のモノリス基材へと適用した。第1の工程において、第1の端部への適用からのコーティングを乾燥させることができ、乾燥させた基材モノリスを180度反転させることができ、同じ手順を、基材モノリスの第1および第2の端部からの適用の間に層の重なり合いが実質的に存在しないように、基材モノリスの上側の第2の端部へと行なうことができる。次いで、得られたコーティング製品を乾燥させ、その後にか焼した。このプロセスを、第2のウォッシュコートコーティング成分にて繰り返し、本発明による触媒(2層)基材モノリスをもたらすことができる。得られたコート済みのモノリス基材を、Pt塩を含む第2の触媒のウォッシュコートでコートし、その後に同じ乾燥および焼成工程を行なった。用いたPtおよびPd塩の量および濃度は、(2層構造における)白金族の金属の総量が2Pt:Pdの比で100gft−3になるように計算した。下側層は、33gft−3のPdおよび63gft−3のPtを含んでおり、上側層は、3gft−3のPtを含んでいた。仕上がった触媒について、10%のH2O、10%のO2、および残りのN2において16時間にわたって800℃で希薄熱水エージングを行なった。
実施例1の触媒を、NOx捕捉部エンジン較正を備えるエンジン管理システム(すなわち、市販の車両はNOx捕捉部およびNOx捕捉部エンジン較正を装備している)を有する試験台に取り付けられた2.0リットルのディーゼルエンジンへと、既存の密着位置(すなわち、エンジンの排気マニホールドの近く)に取り付けた。我々の試験においては、NOx捕捉部を取り外し、DOCで置き換えた。第1の実行において、エンジン動力計を使用し、希薄熱水エージングを行なったDOCの累積のCO変換を欧州MVEG−Bサイクルにおいて試験し、排気ガスの組成をDOCの上流および下流の両方で監視した。このサイクルにおいて「濃いパージ」は生じず、すなわちエンジン管理システムが、触媒に吸着されたNOxを除去および還元するように構成された条件へと切り換わることはなかった。「濃いパージ」は、本発明による触媒を活性化させるために使用され、試験において濃いパージが生じると、結果の比較が難しくなると考えられる。
実施例1において説明したとおりに、本発明による同一の希薄熱水エージングした触媒を作成した。この触媒を、実施例2に使用したエンジンとは異なるが、やはりNOx捕捉部の再生について較正された試験台取り付けの2.0リットルのディーゼルエンジンへと、密着位置に取り付けた。エンジン動力計を使用し、このエンジンを欧州MVEG−B排出物サイクルにて運転し、エンジン出口および触媒の下流の両方における排気ガスのCO含有量を監視した。排気ガスの累積のCO含有量が、図3の上段のグラフに示されており、上側の線が、エンジン出口の排出物におけるCO含有量を示している。この最初の実行におけるCOの排出は、1.04g/kmであった。
Claims (15)
- 希薄燃焼内燃機関と、エンジン管理手段と、エンジンの排気ガスを処理するための排気系とを備えており、前記排気系が、第1のハニカムモノリス基材に配置された第1の酸化触媒を備え、前記第1の酸化触媒は、少なくとも1つの還元可能な酸化物を含む第1の金属酸化物支持体上に支持された白金を含んでおり、前記第1の酸化触媒が、アルカリ金属およびアルカリ土類金属を実質的に含まず、前記エンジン管理手段が、使用時に、前記第1の酸化触媒に接触する排気ガスのラムダ組成を間欠的に調節してラムダ組成を濃くするように構成されている装置。
- 前記少なくとも1つの還元可能な酸化物が、マンガン、鉄、すず、銅、コバルト、またはセリウムで構成されるグループから選択される1つ以上の金属を含む酸化物、複合酸化物、および混合酸化物、ならびに随意により安定化されたこれらの同族体で構成されるグループから選択される、請求項1に記載の装置。
- 前記少なくとも1つの還元可能な酸化物が、MnO2、Mn2O3、Fe2O3、SnO2、CuO、CoO、およびCeO2を含む、請求項2に記載の装置。
- CeO2の安定化された同族体が、ジルコニア、少なくとも1つの非セリウム希土類酸化物、あるいはジルコニアおよび少なくとも1つの非セリウム希土類酸化物の両方を含む、請求項2または3に記載の装置。
- 前記第1の金属酸化物支持体が、バルクの少なくとも1つの還元可能な酸化物または随意により安定化されたその同族体で基本的に構成される、請求項2〜4のいずれか一項に記載の装置。
- 前記少なくとも1つの還元可能な酸化物または随意により安定化されたその同族体が、前記白金とともに前記第1の金属酸化物支持体上に支持される、請求項2〜4のいずれか一項に記載の装置。
- 前記第1の酸化触媒における白金族の金属成分が、10g/ft3超の量で前記モノリス基材上に配置されている、請求項1〜6のいずれか一項に記載の装置。
- 前記第1の酸化触媒が、白金と組み合わせて前記第1の金属酸化物支持体上に支持されたパラジウムを含んでいる、請求項1〜7のいずれか一項に記載の装置。
- 前記第1の酸化触媒が、少なくとも1つの分子ふるいを備えている、請求項1〜8のいずれか一項に記載の装置。
- 前記少なくとも1つの分子ふるいが、銅および/または鉄ならびに少なくとも1つの貴金属を含んでいる、請求項9に記載の装置。
- 前記第1の酸化触媒が、該第1の酸化触媒とは異なる第2の別の酸化触媒と組み合わせられ、該第2の酸化触媒は、第2の金属酸化物支持体上に支持された少なくとも1つの貴金属を含んでいる、請求項1〜10のいずれか一項に記載の装置。
- 前記第1のハニカムモノリス基材と、存在するのであれば第2のハニカムモノリス基材とが、排気ガスから粒子状物質をろ過するための随意により触媒化されたフィルタの上流に配置される、請求項1〜11のいずれか一項に記載の装置。
- 前記第1のハニカムモノリス基材が、チッ素還元剤を用いてチッ素の酸化物を選択的に還元するための触媒を含むモノリス基材の上流に配置される、請求項1〜12のいずれか一項に記載の装置。
- 前記モノリス基材が、貫流モノリス基材である、請求項13に記載の装置。
- 第1の金属酸化物支持体上に支持された白金を含んでおり、ハニカムモノリス基材上に配置され、希薄燃焼内燃機関の排ガス中で経年劣化した第1の酸化触媒の酸化活性を回復させる方法であって、
濃いラムダ組成へと調節された排気ガスに前記第1の酸化触媒を間欠的に接触させるステップを含んでおり、前記第1の金属酸化物支持体が、少なくとも1つの還元可能な酸化物を含んでおり、前記第1の酸化触媒が、アルカリ金属およびアルカリ土類金属を実質的に含んでいない方法。
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- 2011-12-21 CN CN201180058350.8A patent/CN103269775B/zh active Active
- 2011-12-21 KR KR1020137015713A patent/KR101909303B1/ko active IP Right Grant
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- 2011-12-21 DE DE201110089371 patent/DE102011089371B4/de not_active Revoked
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US9140167B2 (en) | 2015-09-22 |
WO2012085572A2 (en) | 2012-06-28 |
RU2013133964A (ru) | 2015-01-27 |
GB2486810B (en) | 2013-09-11 |
DE102011089371B4 (de) | 2013-07-18 |
KR20130132862A (ko) | 2013-12-05 |
WO2012085572A3 (en) | 2012-09-07 |
EP2654929A2 (en) | 2013-10-30 |
EP2654929B1 (en) | 2020-02-12 |
JP6463887B2 (ja) | 2019-02-06 |
US20150375221A1 (en) | 2015-12-31 |
GB201021887D0 (en) | 2011-02-02 |
JP2014510220A (ja) | 2014-04-24 |
KR101909303B1 (ko) | 2018-10-17 |
JP6670273B2 (ja) | 2020-03-18 |
BR112013014585A2 (pt) | 2019-02-19 |
US20130340414A1 (en) | 2013-12-26 |
GB201121961D0 (en) | 2012-02-01 |
DE102011089371A1 (de) | 2012-06-21 |
JP2020076408A (ja) | 2020-05-21 |
RU2577856C2 (ru) | 2016-03-20 |
GB2486810A (en) | 2012-06-27 |
CN103269775B (zh) | 2016-03-02 |
CN103269775A (zh) | 2013-08-28 |
EP3673978A1 (en) | 2020-07-01 |
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