JP6629269B2 - アンモニア生成触媒およびscr触媒を備える排出処理システム - Google Patents
アンモニア生成触媒およびscr触媒を備える排出処理システム Download PDFInfo
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- JP6629269B2 JP6629269B2 JP2017141543A JP2017141543A JP6629269B2 JP 6629269 B2 JP6629269 B2 JP 6629269B2 JP 2017141543 A JP2017141543 A JP 2017141543A JP 2017141543 A JP2017141543 A JP 2017141543A JP 6629269 B2 JP6629269 B2 JP 6629269B2
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- catalyst
- nox
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- lean
- ammonia
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- 239000003054 catalyst Substances 0.000 title claims description 240
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 title claims description 78
- 229910021529 ammonia Inorganic materials 0.000 title claims description 39
- 239000007789 gas Substances 0.000 claims description 72
- 229910052751 metal Inorganic materials 0.000 claims description 50
- 239000002184 metal Substances 0.000 claims description 50
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 38
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 38
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 37
- 239000010949 copper Substances 0.000 claims description 37
- 238000000034 method Methods 0.000 claims description 32
- 230000009467 reduction Effects 0.000 claims description 26
- 229910052802 copper Inorganic materials 0.000 claims description 25
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical group [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 24
- 239000002808 molecular sieve Substances 0.000 claims description 23
- 230000003647 oxidation Effects 0.000 claims description 23
- 238000007254 oxidation reaction Methods 0.000 claims description 23
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 23
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 claims description 22
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- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 claims description 21
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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 5
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- 229910052684 Cerium Inorganic materials 0.000 description 3
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- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 3
- DUFCMRCMPHIFTR-UHFFFAOYSA-N 5-(dimethylsulfamoyl)-2-methylfuran-3-carboxylic acid Chemical compound CN(C)S(=O)(=O)C1=CC(C(O)=O)=C(C)O1 DUFCMRCMPHIFTR-UHFFFAOYSA-N 0.000 description 2
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- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- 238000001694 spray drying Methods 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 1
- 230000019635 sulfation Effects 0.000 description 1
- 238000005670 sulfation reaction Methods 0.000 description 1
- 150000004763 sulfides Chemical class 0.000 description 1
- 229910000601 superalloy Inorganic materials 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 230000001052 transient effect Effects 0.000 description 1
- 229910000314 transition metal oxide Inorganic materials 0.000 description 1
- 230000032258 transport Effects 0.000 description 1
- 230000001960 triggered effect Effects 0.000 description 1
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 description 1
Images
Classifications
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- 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
- F01N3/18—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 methods of operation; Control
- F01N3/20—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 methods of operation; Control specially adapted for catalytic conversion ; Methods of operation or control of catalytic converters
- F01N3/206—Adding periodically or continuously substances to exhaust gases for promoting purification, e.g. catalytic material in liquid form, NOx reducing agents
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y02T10/00—Road transport of goods or passengers
- Y02T10/10—Internal combustion engine [ICE] based vehicles
- Y02T10/12—Improving ICE efficiencies
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Description
NO+I/2O2 → NO2 (1)
硝酸塩としてのNOx吸蔵
2NO2 +MCO3 +1/2O2 → M(NO3)2 +CO2 (2)
NOx放出
M(NO3)2 +2CO → MCO3 +NO2 +NO+CO2 (3)
NOxのN2への還元
NO2 +CO → NO+CO2 (4)
2NO+2CO → N2 +2CO2 (5)
CO + H2O → H2 + CO2 (6a)
2NO + 3H2 + 2CO → 2NH3 + 2CO2 (6b)
基板
本発明のシステムで使用されるLNT触媒組成は、NOx吸着媒および耐火金属酸化物支持体において拡散した白金族金属成分を含む。さらに、LNT触媒組成は、濃密作動期間の間に形成されたNH3の量に大きく影響する、酸素吸蔵成分等の他の成分を任意で含む。
希薄排気において効率的にNOxを処理することが実証された公知のSCR触媒の全てが、LNT触媒の下流での使用に適しているわけではない。例えば、卑金属(例えば銅、鉄)交換されたゼオライト組成(例えばCu−YおよびFe−ベータ)またはバナジウム含有ベースの組成(例えばV2O5/WO3/TiO2/SiO2)は、所望のNH3転換を提供するためには不十分である。これらのSCR触媒は、希薄および濃密LNT作動の間、十分な熱安定性を有していない、または、LNTから生成されたNH3をトラップするために、低いNH3吸蔵を呈する。このため、当該技術は、LNTとの組み合わせにおいて効率的に使用可能なSCR触媒を模索し続けている。
本発明の一実施形態は、CHA結晶構造および約15を超えるシリカ対アルミナのモル比率、ならびに約0.25を超える銅対アルミニウムの原子比率を有するゼオライトを含む触媒に関する。特定の実施形態では、シリカ対アルミナのモル比率は約15〜約256であり、銅対アルミニウムの原子比率は、約0.25〜約0.50である。より特定の実施形態では、シリカ対アルミナのモル比率は約25〜約40である。またさらに特定の実施形態では、シリカ対アルミナのモル比率は約30である。ある特定の実施形態では、銅対アルミニウムの原子比率は約0.30〜約0.50である。特定の実施形態では、銅対アルミニウムの原子比率は約0.40である。特定の実施形態では、シリカ対アルミナのモル比率は、約25〜約40であり、銅対アルミニウムの原子比率は、約0.30〜約0.50である。別の特定の実施形態では、シリカ対アルミナは約30であり、銅対アルミナの原子比率は約0.40である。
SCR触媒が全く存在しない、例1のLNT触媒を作成することにより、排出システムを形成した。
例1で前述したフロースルー触媒のそれぞれから、コアサンプルを採取した。個別のコアサンプルのサイズは、DOCでは、0.75”(D)x0.42”(L)、LNTでは0.75”(D)x1.25”(L)、SCRでは0.75”(D)x0.75”(L)であった。システムサンプルの3セットを、個別の実験用リアクターに、それぞれ組み立てた。実験用リアクター内の各触媒元素の距離は、0.25”であった。この本発明(つまりDOC+LNT+Cu−CHAおよびDOC+LNT+Cu−SAPO)の例1の排出システムおよび比較例2(つまり(DOC+LNTのみ)は、個別に劣化した。劣化過程は、2つのステップで構成される。第一に、触媒システムが、5時間、10%蒸気の流れ空気において、800°Cで劣化された。次いで、触媒システムで、300°Cの硫酸化モード(1gS/L積載)および700°C(LNT床温)の脱硫酸化モード(サイクル10秒希薄および15秒濃密(5分で(λ=0.9)の間)で構成される循環劣化プロトコルが行われた。循環劣化は、40サイクル行った。劣化後、触媒システムを、FTIR分析装置を有するリアクター試験リグで評価した。評価は、120秒の希薄ガスに暴露することを12サイクル行い、次いで、5秒の濃密ガス暴露を行った。希薄ガスは、200ppmNO、5%CO、2.5%H2O、10%O2およびバランスN2で構成される。濃密ガス(λ=0.95)は、2.36%CO、0.78%H2、0.95%O2、5%CO2、5%H2O5、1500ppmC3H6バランスN2を含んでいた。試験時の空間速度は、60,000時間-1(LNT容量に基づく)で一定に保たれた。NH3形成のパーセント劣化は、試験の間中監視され、試験内の全NOx入力に基づくサイクル平均数として報告された。システムのNOxトラップ能力は、12回目の濃密露出の終了後に計測され、80%サイクルNOx転換に達すると、システムから除去されたNOx量として表された。
例4のLNT触媒を作成することにより、およびフィルタのSCR触媒の下流の効果を示すために、フィルタ上に下流SCR触媒が存在する場合に、排出システムが形成された。
実施例4の排出システムおよび比較のための実施例5が、新欧州ドライブサイクル(NEDC)条件の過渡エンジン試験セルで試験された。当該技術のエンジンの6−シリンダ状態が使用された。図6は、エンジン試験中において蓄積されたNOx排出を示し、ここで、エンジン速度は最も底部のラインによって示され、NOx排出は、(a)エンジンアウト、(b)NOxトラップ後、および(c)SCRF後において計測される。図6に示されるように、例4の組み合わせられたシステムの全NOx転換は約80%であり、これは、試験サイクルの終了時においてライン(c)上のおよそ2.67gからおよそ0.56gへ還元された蓄積されたNOx排出によって示され、一方で、比較例5のシステムは約68%であり、これは、試験サイクルの終了時においてライン(b)上のおよそ2.67gからおよそ0.86gへ還元される蓄積されたNOx排出によって示される。
Claims (20)
- ディーゼルエンジンまたは希薄燃焼ガソリンエンジンの排気流の排出処理システムであって、
担体上に設けられた少なくともNOx吸着媒と、担体上に設けられた窒素種の酸化及び還元を促進する1種以上の白金族金属とを含む、2元触媒機能を有する上流アンモニア生成触媒;及び
CHA結晶構造を有する分子篩を含む下流SCR触媒を含む排出処理システム。 - 前記アンモニア生成触媒は、希薄エンジン作動時にNOxを吸着することができ、濃密エンジン作動時においてNOxをN2に還元し、NOxを脱着し、NH3を生成することができる希薄NOxトラップ(LNT)触媒材料を含む請求項1に記載の排出処理システム。
- 前記少なくとも1種のNOx吸着媒が、アルカリ土類元素、希土類元素、及びこれらの組み合わせからなる群から選択される元素を含む請求項1に記載の排出処理システム。
- 前記NOx吸着媒は、前記担体上の第1の層として存在し、前記窒素種の酸化および還元を促進する前記1種以上の白金族金属は、前記担体上の第2の別の層として存在する、請求項1に記載の排出処理システム。
- 前記NOx吸着媒は、担体上のアンダーコートウォッシュコート層として存在し、窒素種の酸化および還元を促進する前記1種以上の白金族金属は、トップウォッシュコート層として存在する請求項4に記載の排出処理システム。
- 前記トップウォッシュコート層がアルカリ土類成分を実質的に含まない請求項5に記載の排出処理システム。
- 二元触媒機能を有するアンモニア生成触媒が、フロースルーモノリスである担体上に配置される請求項1に記載の排出処理システム。
- 前記窒素種の酸化及び還元を促進する前記1種以上の白金族金属が、50/(0.30483)〜200/(0.30483)g/m3(50〜200g/ft3)の範囲の量で存在する請求項1に記載の排出処理システム。
- 前記二元触媒機能を有する上流アンモニア生成触媒が、少なくとも1種のアルカリ土類元素及び少なくとも1種の白金族金属を担持する1種以上の耐火金属酸化物を含むウォッシュコート層を含む、請求項1に記載の排出処理システム。
- 前記1種以上の耐火金属酸化物が、アルミナ、セリア、ジルコニア、及びこれらの組み合わせからなる群から選択される請求項9に記載の排出処理システム。
- 前記二元触媒機能を有する上流アンモニア生成触媒が、アルミナ、セリア、少なくとも1種の白金族金属、並びに酸化バリウム及び酸化マグネシウムの少なくとも1種を含むウォッシュコート層を含む請求項1に記載の排出処理システム。
- 前記SCR触媒は、0.5/(25.43)〜2.5/(25.43)g/mm3(0.5〜2.5g/in3)の範囲の量で存在する請求項1に記載の排出処理システム。
- 前記CHA結晶構造を有する分子篩が、約15〜約256のシリカ対アルミナのモル比を有する請求項1に記載の排出処理システム。
- 前記CHA結晶構造を有する分子篩が、卑金属交換物質である請求項1に記載の排出処理システム。
- 前記CHA結晶構造を有する分子篩が、約0.30〜約0.50の卑金属対アルミナのモル比を有する、請求項14に記載の排出処理システム。
- 前記CHA結晶構造を有する分子篩が、担体上に配置された銅チャバサイト(CuCHA)又は担体上に配置された銅SAPO(CuSAPO)である請求項1に記載の排出処理システム。
- 前記下流の担体は、長手方向に延伸する壁によって境界を示され画定されて形成された複数の長手方向に延伸する通路を有するウオールフローフィルタを備え、前記通路は、開いた流入端および閉じた流出端を有する流入通路と、閉じた流入端および開いた流出端を有する流出通路とを備えている請求項16に記載の排出処理システム。
- 前記ウオールフローフィルタは、軸方向長さの約10%〜100%の範囲で前記SCR触媒によって被覆されている請求項17に記載の排出処理システム。
- ディーゼルエンジンまたは希薄燃焼ガソリンエンジンからの排気ガス流内のNOxをN2へ転換するための方法であって、請求項1に記載の排出処理システムを通して前記排気ガス流を送ることを含む、転換方法。
- (a)前記排気ガス流からのNOxを吸着するために、希薄期間にNOxを含む前記排気ガス流を、2元触媒機能を有する上流アンモニア生成触媒に接触させる工程と、
(b)濃密期間に濃密ガス流を提供するために、前記排気流の空気/燃料比率を周期的に変える工程と、
(c)前記吸着されたNOxの一部をアンモニアに還元するために、前記濃密ガス流を前記2元触媒機能を有する上流アンモニア生成触媒に接触させ、前記下流SCR触媒にアンモニアを吸着させる工程と、
(d)次いで、前記下流SCR触媒に吸着されたアンモニアと前記排気ガス内のNOxを前記SCR触媒を用いて反応させる工程と、を含み、且つ
前記SCR触媒はアンモニアの増加を低減するのに有効である請求項19に記載の方法。
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