JP2020514039A - アンモニアスリップ触媒を有する触媒ウォールフローフィルタ - Google Patents
アンモニアスリップ触媒を有する触媒ウォールフローフィルタ Download PDFInfo
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- JP2020514039A JP2020514039A JP2019551342A JP2019551342A JP2020514039A JP 2020514039 A JP2020514039 A JP 2020514039A JP 2019551342 A JP2019551342 A JP 2019551342A JP 2019551342 A JP2019551342 A JP 2019551342A JP 2020514039 A JP2020514039 A JP 2020514039A
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- 230000003197 catalytic effect Effects 0.000 title claims abstract description 52
- 239000000758 substrate Substances 0.000 claims abstract description 121
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 82
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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 claims description 50
- 239000011148 porous material Substances 0.000 claims description 47
- 238000000034 method Methods 0.000 claims description 39
- 239000010457 zeolite Substances 0.000 claims description 38
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 34
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- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- 229910001930 tungsten oxide Inorganic materials 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- 229910001935 vanadium oxide Inorganic materials 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
- 229910052726 zirconium Inorganic materials 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
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Abstract
Description
4NO+4NH3+O2→4N2+6H2O
2NO2+4NH3+O2→3N2+6H2O
NO+NO2+2NH3→2N2+3H2O
第1の複数のチャネルは、第1の端面で開いており、第2の端面で閉じており、第2の複数のチャネルは、第2の端面で開いており、第1の端面で閉じており、
モノリスフィルタは、チャネルを規定する表面を有し、且つフィルタ長さ未満の距離にわたって第1の端面から第2の端面へ向かって縦方向に延びる第1のゾーンと、フィルタ長さ未満の距離にわたって第2の端面から第1の端面へ向かって縦方向に延びる第2のゾーンとを有する多孔質基材を含み、
第1のゾーンは、多孔質基材全体に分布する第1のSCR触媒を含み、第2のゾーンは、多孔質基材全体に分布するアンモニア酸化触媒を含み、
第2のSCR触媒は、多孔質基材の第2のゾーンの表面を覆う層に位置する。第2のSCR触媒は、(1)第2のゾーンの多孔質基材の表面を覆う層にのみ存在し得る(すなわち、多孔質基材全体に分布していない)(オンウォール)か、又は(2)第2のゾーンの多孔質基材の表面を覆う層(オンウォール)と、第2のゾーンの多孔質基材の実質的に全て又は一部(例えば壁中)(インウォール)とに存在し得る。第2のSCR触媒は、第2のゾーンの多孔質基材の全て又は一部に存在するとき、アンモニア酸化触媒の全て又は一部と共に存在し得る。
(a)間に縦方向を規定する第1の端面及び第2の端面並びに縦方向に延びる第1及び第2の複数のチャネルを有する多孔質基材を提供することであって、第1の複数のチャネルが、第1の端面で開いており、第2の端面で閉じており、第2の複数のチャネルが、第2の端面で開いており、第1の端面で閉じている、多孔質基材を提供する、こと;
(b)第1のSCR触媒を含むウォッシュコートを多孔質基材に選択的に浸透させることにより、第1のゾーンを形成すること、
(c)アンモニア酸化触媒を含むウォッシュコートを多孔質基材に選択的に浸透させることにより、第2のゾーンの一部を形成すること、
(c)第2の複数のチャネルの壁がコーティングにより覆われている第2のゾーンのアンモニア酸化触媒上に第2のSCR触媒のコーティングを形成すること、
を含む触媒ウォールフローモノリスフィルタの製造のための方法に関し、
工程(b)が工程(c)の前に実施され得るか、又は工程(c)が工程(b)の前に実施され得る。
SCR触媒は、卑金属の酸化物、モレキュラーシーブ、金属交換モレキュラーシーブ又はこれらの混合物であり得る。卑金属は、セリウム(Ce)、クロム(Cr)、コバルト(Co)、銅(Cu)、鉄(Fe)、マンガン(Mn)、モリブデン(Mo)、ニッケル(Ni)、タングステン(W)、バナジウム(V)、及びこれらの混合物からなる群より選択され得る。アルミナ、シリカ、ジルコニア、チタニア、セリア及びそれらの組み合わせなどの耐火性金属酸化物上に担持されたバナジウムからなるSCR組成物は、周知であり、自動車用途で商業的に広く使用されている。典型的な組成物は、米国特許第4010238号及び同第4085193号に記載されており、これらの全内容は参照により本明細書に援用される。商業的に、特に自動車用途において使用される組成物は、TiO2であってその上にWO3及びV2O5が各々5〜20重量%及び0.5〜6重量%の範囲の濃度で分散されているTiO2を含む。これらの触媒は、結合剤及び促進剤として作用する、SiO2及びZrO2などの他の無機材料を含んでもよい。
酸化触媒は、貴金属又はその混合物を含み得る。好ましくは、貴金属は、金、銀、白金、パラジウム、ルテニウム若しくはロジウム、又はそれらの組み合わせである。より好ましくは、貴金属は、白金又はパラジウム又は白金とパラジウムの組み合わせである。
(a)第1の端面と第2の端面との間に縦方向を規定する第1の端面及び第2の端面並びに縦方向に延びる第1及び第2の複数のチャネルを有する多孔質基材を提供することであって、第1の複数のチャネルが、第1の端面で開いており、第2の端面で閉じており、第2の複数のチャネルが、第2の端面で開いており、第1の端面で閉じている、多孔質基材を提供すること;
(b)第1のSCR触媒を含むウォッシュコートを多孔質基材に選択的に浸透させることにより、第1のゾーンを形成すること、
(c)アンモニア酸化触媒を含むウォッシュコートを多孔質基材に選択的に浸透させることにより、第2のゾーンの一部を形成すること、
(d)第2の複数のチャネルの壁がコーティングにより覆われている第2のゾーンのアンモニア酸化触媒上に第2のSCR触媒のコーティングを形成すること、
を含む方法が提供され、ここで、工程(b)は工程(c)の前に実施され得るか、又は工程(c)は工程(b)の前に実施され得る。
初めに、アルミナ上白金を含む酸化触媒を含むウォッシュコートを、一端からフィルタ長さの10%にわたって置くことにより、フィルタの壁中のアンモニア酸化触媒を有するフィルタを、SiCフィルタ基材(300cpsi、12milの壁厚)で調製した。Ptローディングは、6g/ft3であった。その後、アルミナ上Ptを含むウォッシュコートを含むフィルタを乾燥させ、500℃で1時間焼成した。その後、銅チャバザイト(Cu−CHA)、アルミナ及びレオロジー調整剤を含むウォッシュコートを塗布することにより、SCR層をアンモニア酸化触媒を含有しなかったフィルタ長さの90%にわたって置いた。その後、SCRウォッシュコートを含む層をアンモニア酸化触媒上に置いた。Cu−CHAのローディングは1.71g/in3であった。SCRウォッシュコートを含むフィルタを乾燥させ、その後500℃で1時間焼成した。フィルタを800℃で16時間熱水的にエイジングした。
初めに、銅チャバザイト(Cu−CHA)、アルミナ及びレオロジー調整剤を含むSCRウォッシュコートウォッシュコートをフィルタに置いてSCR層を形成することにより、フィルタの壁上のアンモニア酸化触媒を有するフィルタを、SiCフィルタ基材(300cpsi、12milの壁厚)で調製した。Cu−CHAのローディングは1.71g/in3であった。SCRウォッシュコートを含むフィルタを乾燥させ、その後500℃で1時間焼成した。アルミナ上白金を含む酸化ウォッシュコートを、フィルタの一端からフィルタ長さの20%にわたってSCR触媒上に塗布することによって、SCR触媒上の酸化触媒の層を形成した。Ptローディングは、3g/ft3であった。SCR触媒の長さの20%にわたって酸化触媒の層を有するフィルタを乾燥させ、その後500℃で1時間焼成した。フィルタを800℃で16時間熱水的にエイジングした。
3l V6エンジンを備えた自動車で実施例1及び2の試料を試験した。ディーゼル酸化触媒(DOC)は、実施例1又は2の試料の前に位置していた。1:2のアンモニア:NOxの比(アルファ)で車両を操作した。エンジンの負荷を調整して、フィルタの入口温度を610℃にし、その後、入口温度を610℃で約20分間維持した。その後、負荷を減少させ、入口温度を420℃に低下させた。入口温度を420℃で約20分間維持した。入口温度が以下の表に示される温度で維持されるように、エンジンの負荷を数回減少させた。温度を定常状態で維持しながら、以下に示すように、ガスの流れ及び排気中の様々な成分について測定した。
Claims (30)
- 排出処理システムにおける使用のための触媒ウォールフローモノリスフィルタであって、第1の端面、第2の端面、第1の端面から第2の端面までの距離によって規定されるフィルタ長さ、第1の端面と第2の端面との間の縦方向、並びに縦方向に延びる第1及び第2の複数のチャネルを含み、
第1の複数のチャネルが、第1の端面で開いており、第2の端面で閉じており、第2の複数のチャネルが、第2の端面で開いており、第1の端面で閉じており、
モノリスフィルタが、チャネルを規定する表面を有し、且つフィルタ長さ未満の距離にわたって第1の端面から第2の端面へ向かって縦方向に延びる第1のゾーンと、フィルタ長さ未満の距離にわたって第2の端面から第1の端面へ向かって縦方向に延びる第2のゾーンとを有する多孔質基材を含み、
第1のゾーンが、多孔質基材全体に分布する第1のSCR触媒を含み、第2のゾーンが、多孔質基材全体に分布するアンモニア酸化触媒を含み、第2のSCR触媒が、多孔質基材の第2のゾーンの表面を覆う層に位置している、
触媒ウォールフローモノリスフィルタ。 - 第2のSCR触媒が、第2のゾーンの多孔質基材の表面を覆う層にのみ存在している、請求項1に記載の触媒ウォールフローモノリスフィルタ。
- 第2のSCR触媒が、第2のゾーンの多孔質基材の表面を覆う層及び第2のゾーンの多孔質基材の全て又は一部に存在している、請求項1に記載の触媒ウォールフローモノリスフィルタ。
- 第2のSCR触媒が、第2のゾーンの多孔質基材の表面を覆う層及び第2のゾーンの多孔質基材の全てに存在している、請求項3に記載の触媒ウォールフローモノリスフィルタ。
- 第2のSCR触媒が、多孔質基材の第2のゾーンの表面を覆う層及び第2のゾーンの多孔質基材の一部に存在している、請求項3に記載の触媒ウォールフローモノリスフィルタ。
- 第1のゾーンにおいて、第1のSCR触媒が第1又は第2の複数のチャネルの表面を覆っていない、請求項1から5のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 第1のSCR触媒が第2のSCR触媒と同一である、請求項1から6のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 第2のSCR触媒が第2のSCR触媒とは異なる、請求項1から7のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 第1のSCR触媒及び第2のSCR触媒の少なくとも一つが、小細孔モレキュラーシーブ、好ましくはゼオライト、中細孔モレキュラーシーブ、好ましくはゼオライト、大細孔モレキュラーシーブ、好ましくはゼオライト、又は卑金属を含む、請求項1から8のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 小細孔モレキュラーシーブが、AEI、AFT、CHA、DDR、EAB、ERI、GIS、GOO、KFI、LEV、LTA、MER、PAU、VNI及びYUGから、好ましくはAEI、CHA及びLTAからなる群より独立して選択される骨格構造を有する、請求項9に記載の触媒ウォールフローモノリスフィルタ。
- 第1のSCR触媒及び第2のSCR触媒の少なくとも一つが銅ベータゼオライトを含む、請求項9に記載の触媒ウォールフローモノリスフィルタ。
- 第1のSCR触媒及び第2のSCR触媒の少なくとも一つが、Wを含浸させたCeO2、Wを含浸させたCeZrO2、及びFeとWを含浸させたZrO2を含む、請求項1から4のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 第1のSCR触媒が、好ましくは、AEI、AFT、CHA、DDR、EAB、ERI、GIS、GOO、KFI、LEV、LTA、MER、PAU、VNI及びYUGの構造ファミリーから、より好ましくはAEI、CHA及びLTAからなる群より選択される骨格構造を有する小細孔モレキュラーシーブを含む、請求項1から12のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 第2のSCR触媒が、大細孔モレキュラーシーブ、好ましくは銅ベータゼオライトであるか、又はWを含浸させたCeO2、Wを含浸させたCeZrO2、若しくはFeとWを含浸させたZrO2から選択される非ゼオライト材料である、請求項1から13のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 縦方向における第2のゾーンの長さ対第1のゾーンの長さの比が、1:20から1:5、好ましくは約1:9である、請求項1から14のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 第2のSCR触媒が、モノリス基材の長さの約10%から約50%、約10%から約45%、約10%から約40%、約10%から約35%、約10%から約30%、約10%から約25%、又は約10%から約20%で存在する、請求項1から11のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 酸化触媒が、貴金属、好ましくは白金、パラジウム又はそれらの組み合わせを含む、請求項1から16のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- フィルタが、100cpsiから600cpsi(15.5cpscmから93cpscm)のセル密度を有する、請求項1から17のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 隣接するチャネル間の基材の平均最小厚さが6から20mil(0.015から0.05cm)である、請求項1から18のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 第2のゾーンの第2のSCR触媒が、10μmから80μmの厚さを有するコーティングとして第2の複数のチャネルの壁を覆っている、請求項1から19のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 第1のゾーンと第2のゾーンとの間に位置する第3のゾーンであって、多孔質基材全体に分布している第1のSCR触媒と、多孔質基材の表面を覆い、多孔質基材全体に分布していない層に位置する第2のSCR触媒とを含む、第3のゾーンをさらに含む、請求項1から20のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 第3のゾーンが、モノリス基材の長さの最大10%、好ましくは最大5%の長さを有する、請求項21に記載の触媒ウォールフローモノリスフィルタ。
- (a)第1のゾーンと第2のゾーン;(b)第1のゾーンと第3のゾーン;又は(c)第3のゾーンと第2のゾーンの少なくとも一部の間に間隙をさらに含む、請求項1から22のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- (a)第1のゾーンと第2のゾーン;(b)第1のゾーンと第3のゾーン;又は(c)第3のゾーンと第2のゾーンの少なくとも一部の間に間隙がない、請求項1から23のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 触媒ウォールフローモノリスが、第2のゾーンのコーティングとして第2のSCR触媒を含まないウォールフローフィルタと比較して、NOx変換の改善及びN2O形成の減少の少なくとも一つを提供する、請求項1から24のいずれか一項に記載の触媒ウォールフローモノリスフィルタ。
- 燃焼排気ガスの流れを処理するための排出処理システムであって、請求項1から25のいずれか一項に記載の触媒ウォールフローモノリスフィルタを含み、第1の端面が第2の端面の上流にある、排出処理システム。
- 第2のゾーンのコーティングとして第2のSCR触媒を含まないウォールフローフィルタと比較して、NOx変換の改善及びN2O形成の減少の少なくとも一つを提供する、請求項26に記載の排出処理システム。
- 請求項1から25のいずれか一項に記載の触媒ウォールフローモノリスフィルタの製造のための方法であって、
(a)第1の端面と第2の端面との間に縦方向を規定する第1の端面及び第2の端面並びに縦方向に延びる第1及び第2の複数のチャネルを有する多孔質基材を提供することであって、第1の複数のチャネルが、第1の端面で開いており、第2の端面で閉じており、第2の複数のチャネルが、第2の端面で開いており、第1の端面で閉じている、多孔質基材を提供すること;
(b)第1のSCR触媒を含むウォッシュコートを多孔質基材に選択的に浸透させることにより、第1のゾーンを形成すること、
(c)アンモニア酸化触媒を含むウォッシュコートを多孔質基材に選択的に浸透させることにより、アンモニア酸化触媒を含む第2のゾーンの一部を形成すること、及び
(d)第2の複数のチャネルの壁がコーティングにより覆われている第2のゾーンのアンモニア酸化触媒上に第2のSCR触媒のコーティングを形成すること、
を含み、
工程(b)が工程(c)の前に実施され得るか、又は工程(c)が工程(b)の前に実施され得る、方法。 - NOxを含む燃焼排気ガスの流れを処理するための方法であって、排気流を請求項1から25のいずれか一項に記載のモノリスに通すことを含み、第1の端面が第2の端面の上流にある、方法。
- 第2のゾーンのコーティングとして第2のSCR触媒を含まないウォールフローフィルタと比較して、NOx変換の改善及びN2O形成の減少の少なくとも一つ、請求項29に記載の方法。
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DE102018106415A1 (de) | 2018-09-20 |
US10369555B2 (en) | 2019-08-06 |
CN110573236A (zh) | 2019-12-13 |
BR112019019548A2 (pt) | 2020-04-22 |
KR20190126903A (ko) | 2019-11-12 |
WO2018172930A1 (en) | 2018-09-27 |
GB201804369D0 (en) | 2018-05-02 |
KR102532962B1 (ko) | 2023-05-17 |
GB2562160A (en) | 2018-11-07 |
RU2019133124A (ru) | 2021-04-21 |
RU2755135C2 (ru) | 2021-09-13 |
EP3600620A1 (en) | 2020-02-05 |
JP7110224B2 (ja) | 2022-08-01 |
US20180264446A1 (en) | 2018-09-20 |
RU2019133124A3 (ja) | 2021-04-21 |
GB2562160B (en) | 2021-06-23 |
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