JP2022534180A - 触媒化ガソリン微粒子フィルタ - Google Patents
触媒化ガソリン微粒子フィルタ Download PDFInfo
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- JP2022534180A JP2022534180A JP2021563009A JP2021563009A JP2022534180A JP 2022534180 A JP2022534180 A JP 2022534180A JP 2021563009 A JP2021563009 A JP 2021563009A JP 2021563009 A JP2021563009 A JP 2021563009A JP 2022534180 A JP2022534180 A JP 2022534180A
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- JP
- Japan
- Prior art keywords
- particulate filter
- catalyzed
- layer
- alumina
- ceria
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- 239000010410 layer Substances 0.000 claims description 88
- 239000000463 material Substances 0.000 claims description 83
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- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 50
- 239000000203 mixture Substances 0.000 claims description 42
- 239000007789 gas Substances 0.000 claims description 37
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- 229910052751 metal Inorganic materials 0.000 claims description 21
- 239000002184 metal Substances 0.000 claims description 21
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 claims description 20
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 claims description 20
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- 229910052727 yttrium Inorganic materials 0.000 description 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
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Abstract
Description
本発明は、ガソリンエンジンからの排気ガス用の触媒化微粒子フィルタに関するものである。触媒化微粒子フィルタは、効率的なフィルタと併せて、改善された触媒効率を提供する。
(1) ガソリン微粒子フィルタ(GPF)と、
(2) GPF表面の入口側、出口側、又は両側の上又は中に被覆された主触媒層であって、第1の組成物を含み、該第1の組成物が、第1の支持体材料及び第1の白金族金属(PGM)を含む、主触媒層と、
(3) GPF表面の入口側、出口側、又は両側の上又は中に置かれた副次的な機能性材料層であって、第2の組成物を含む、副次的触媒層と
を含み、
(4) 主触媒層が、副次的な機能性材料層よりも高い担持量を有し、
(5) 副次的な機能性材料層が主触媒層の上に置かれ、又は主な触媒材料層が副次的な機能性層の上に置かれている。
触媒材料を有するガソリン微粒子フィルタを、入口側からの被覆と出口側からの被覆との二重被覆を用いて調製した。先行技術の触媒複合体は、ガソリン微粒子フィルタに被覆して、フィルタに捕捉された粒子状物質を低温で酸化し、窒素酸化物、一酸化炭素、及び炭化水素を低減するためのものであり、この複合体は白金、パラジウム、及びロジウムを含有し、貴金属の合計担持量は16.5g/ft3、そしてPt/Pd/Rhの比率は5/6.5/5であった。基材は、体積が2.0L(122in3)、セル密度が1平方インチ当たり300セル、壁厚が約200μm、多孔度が63%、そして水銀圧入測定による平均細孔径が19μmであった。この被覆は次のようにして調製した。
触媒材料を有するガソリン微粒子フィルタを、出口側から被覆された主触媒層と、出口側から被覆された副次的な機能性材料層との二重被覆を用いて調製した。触媒複合体は、白金、パラジウム、及びロジウムを含有し、貴金属の合計担持量は16.5g/ft3、そしてPt/Pd/Rhの比率は5/6.5/5であった。基材は、体積が2.0L(122in3)、セル密度が1平方インチ当たり300セル、壁厚が約200μm、多孔度が63%、そして水銀圧入測定による平均細孔径が19μmであった。この被覆は次のようにして調製した。
副次的な機能性材料層を入口側から施与した実施例2に記載の触媒化ガソリン微粒子フィルタを、粒子径の90%が11.7ミクロン、50%が4.2ミクロン、及び10%が1.4ミクロンになるまで乾式粉砕した。副次的な機能性材料層の担持量は0.26g/in3であった。
途中まで被覆された触媒フィルタとしての実施例1による触媒化ガソリン微粒子フィルタ。
実施例1~4によるガソリン微粒子フィルタをSGE1.5Lターボガソリン直噴エンジンの後の第1位置に置くことにより、これらの触媒化フィルタがガス相汚染物質(未燃焼のHC、CO及びNOx)を変換する能力を評価した(WLTC試験)。結果を図1に示す。副次的な機能性材料層を施与した触媒化ガソリン微粒子フィルタは、3つのカテゴリーの汚染物質すべて、特にHC及びCOの変換の大幅な改善を示した。
触媒材料を有するガソリン微粒子フィルタを、出口側から被覆された主触媒層と、出口側から被覆された副次的な機能性材料層との二重被覆を用いて調製した。触媒複合体は、白金及びパラジウムを含有し、貴金属の合計担持量は6.25g/ft3、そしてPt/Pd/Rhの比率は4/1/0であった。基材は、体積が2.5L(151in3)、セル密度が1平方インチ当たり200セル、壁厚が約200μm、多孔度が55%、そして水銀圧入測定による平均細孔径が9μmであった。この被覆は次のようにして調製した。
主触媒層のスラリーを、粒子径の90%が5ミクロンになるまで粉砕した、実施例6に記載の触媒化ガソリン微粒子フィルタ。
触媒材料を有するガソリン微粒子フィルタを、入口側からの単一を用いて調製した。触媒複合体は白金及びパラジウムを含有し、貴金属の合計担持量は6.25g/ft3、そしてPt/Pd/Rhの比率は4/1/0であった。基材は、体積が2.5L(151in3)、セル密度が1平方インチ当たり200セル、壁厚が約200μm、多孔度が55%、そして水銀圧入測定による平均細孔径が9μmであった。この被覆は次のようにして調製した。
SGE1.5Lターボガソリン直噴エンジンの後の第1位置において、実施例6~8がガス相汚染物質を変換する能力及び新鮮な状態(0km、又は箱から出した状態)での濾過効率を評価した(WLTC試験;PNエンジン出力=3.5×1012#/km)。結果をそれぞれ図3及び図4に示す。これらの実施例では、同様の新鮮な濾過効率が観察され、主触媒層と副次的な機能性材料層の両方を有する触媒化フィルタ(実施例6及び7)は、粉末のみを担持したサンプル(実施例8)よりも有意に良好なTWC活性を示した。
触媒材料を有するガソリン微粒子フィルタを、入口側からの単一被覆を用いて調製した。先行技術の三元変換(TWC)触媒複合体は、パラジウム及びロジウムを含有し、貴金属の合計担持量は7g/ft3、そしてPt/Pd/Rhの比率は0/2/5であった。基材は、体積が2.5L(151in3)、セル密度が1平方インチ当たり300セル、壁厚が約200μm、多孔度が63%、そして水銀圧入測定による平均細孔径が19μmであった。この被覆は次のようにして調製した。
先行技術の三元変換(TWC)触媒複合体が主触媒層であり、追加の副次的な機能性材料層がフィルタの入口側内に担持された、実施例10による触媒化ガソリン微粒子フィルタ。
副次的な機能性材料層の担持量が0.041g/in3であった、実施例11に記載の触媒化ガソリン微粒子フィルタ。
副次的な機能性材料層の担持量が0.024g/in3であった、実施例11に記載の触媒化ガソリン微粒子フィルタ。
施与した副次的な機能性層が高表面積のガンマアルミナである、実施例11と同様に調製した触媒化ガソリン微微粒子フィルタ。アルミナは、90%が16ミクロン、50%が6.9ミクロン、10%が2.0ミクロンの粒子径に乾式粉砕したもので、1000℃の空気中で4時間か焼した後の比表面積(BETモデル、77K窒素吸着測定)は76m2・g-1であった。副次的な機能性材料層の担持量は0.066g/in3であった。
実施例11と同様に調製した触媒化ガソリン微粒子フィルタであって、施与した副次的な機能性層が高表面積のガンマアルミナであった。アルミナは、粒子径の90%が25.4ミクロン、50%が10.9ミクロン、10%が2.4ミクロンになるまで乾式粉砕し、1000℃の空気中で4時間か焼した後のその比表面積(BETモデル、77K窒素吸着測定)は75m2・g-1であった。副次的な機能性材料層の担持量は0.066g/in3であった。
実施例11と同様に調製した触媒化ガソリン微粒子フィルタであって、施与した副次的な機能性層がポリビニルアルコールの粉末をさらに含んでいた。ポリビニルアルコールPVA-1788は、粒子径が230メッシュの微細な粉末として得られた。このPVA粉末を、乾式粉砕した高表面積のガンマアルミナと1:5の割合の質量比で予備混合した。この混合粉末をさらにガス担体と混合し、室温で部品に吹き込んだ。ガス担体の流量は575kg/時間であった。副次的な機能性材料層の総搭載量は0.079g/in3であった。
第1位置において(SGE1.5Lターボガソリン直噴エンジン;WLTC試験;PNエンジン出力=3.5×1012#/km)、実施例10~16の新鮮な状態(0km、又は箱から出した状態)での濾過効率を測定した。結果を図5に示す。副次的な機能性材料層を施与した触媒化ガソリン微粒子フィルタは、副次的な機能性材料層を施与していない先行技術のフィルタと比較して、濾過効率の著しい増加を示した。注目すべきは、濾過効率の増加は、機能性層の担持量が0.024g/in3と低いときにすでに非常に顕著なことである(+24%、実施例10対13)。さらに、本発明の実施態様による実施例の濾過効率は、実施例11及び12で示されるように、副次的な機能性材料層をより高い担持量で施与することによってさらに向上する。機能層の最適化された粒子径分布は、実施例11、14及び15によって実証され、ここでは、粒子径D90を25μm~16μm、さらに5μmに低減することで、より高い濾過効率(FFE)が達成された。有機材料を添加しても(実施例16)、本実施例に従って調製された触媒化ガソリン微粒子フィルタは、その高い濾過効率を維持する。
Claims (16)
- (1) ガソリン微粒子フィルタ(GPF)と、
(2) 前記GPF表面の入口側、出口側、又は両側の上又は中に被覆された主触媒層であって、第1の組成物を含み、前記第1の組成物が、第1の支持体材料及び第1の白金族金属(PGM)を含む、前記主触媒層と、
(3) 前記GPF表面の入口側、出口側、又は両側の上又は中に置かれた副次的な機能性材料層であって、第2の組成物を含む、前記副次的触媒層と
を含み、
(4) 前記主触媒層が、前記副次的な機能性材料層よりも高い担持量を有し、
(5) 前記副次的な機能性材料層が前記主触媒層の上に置かれ、又は前記主な触媒材料層が前記副次的な機能性層の上に置かれている、ガソリンエンジンからの排気ガス用の触媒化微粒子フィルタ。 - 前記第2の組成物が、第2の支持体材料及び第2の白金族金属を含む、請求項1に記載の触媒化微粒子フィルタ。
- 前記第1及び第2の支持体材料が、アルミナ、ジルコニア、セリア、シリカ、チタニア、セリア以外の希土類金属酸化物、及びこれらの混合物からなる群から独立して選択される、請求項2に記載の触媒化微粒子フィルタ。
- 前記第1及び第2のPGMが、白金(Pt)、パラジウム(Pd)、ロジウム(Rh)、及びこれらの混合物からなる群から独立して選択される、請求項2又は3に記載の触媒化微粒子フィルタ。
- 前記第2のPGMが、Pt、又はPt及びPdであり、前記第2のPGMが、触媒的に有効な量で存在して、排気ガス中のNOx、CO及び炭化水素をN2、CO2及びH2Oに変換し、且つガソリン微粒子フィルタに捕捉された粒子状物質の酸化を引き起こす、請求項4に記載の触媒化微粒子フィルタ。
- 前記第1のPGMがRh、又はRh及びPdであり、前記第1のPGMが、触媒的に有効な量で存在して、排気ガス中のNOx、CO及び炭化水素をN2、CO2及びH2Oに変換する、請求項4又は5に記載の触媒化微粒子フィルタ。
- 前記第2の組成物が、セリア、ジルコニア、酸化ストロンチウム、炭酸ストロンチウム、硫酸ストロンチウム、酸化バリウム、炭酸バリウム、硫酸バリウム、酸化マンガンのうちの少なくとも1つを含む、請求項1に記載の触媒化微粒子フィルタ。
- 前記第2の組成物が有する、1000℃の空気中で4時間か焼した後の比BET表面積が、77K窒素収着評価により、5~200m2・g-1の範囲、好ましくは7~100m2・g-1の範囲、及びより好ましくは10~70m2・g-1の範囲である、請求項7に記載の触媒化微粒子フィルタ。
- 前記第2の組成物が、アルミナ、水和アルミナ、又はドープしたアルミナをさらに含み、ドーパントが、セリア、ジルコニア、酸化ストロンチウム、炭酸ストロンチウム、硫酸ストロンチウム、酸化バリウム、炭酸バリウム、硫酸バリウム、酸化マンガンのうちの少なくとも1つである、請求項8に記載の触媒化微粒子フィルタ。
- 前記第2の組成物が、酢酸、シュウ酸、クエン酸、酒石酸、フマル酸、乳酸、リンゴ酸、マレイン酸、ヘキサノール、オクタノール、デカノール、セルロース、ヒドロキシルエチルセルロース、メチルヒドロキシエチルセルロース、デンプン、ポリエチレン、ポリプロピレン、ポリスチレン、ポリ(オキシエチレン)、ポリ(エチレンテレフタレート)、ポリ(ブチレンテレフタレート)、ポリ塩化ビニル、ポリビニルアルコール、ポリビニルピロリドン、ポリメチルメタクリレート、ポリアミド、ポリカーボネート、及びポリウレタンからなる群のうちの1つ以上から選択される有機材料をさらに含む、請求項1から9のいずれか1項に記載の触媒化微粒子フィルタ。
- 前記主触媒層が、10~170g/L、好ましくは25~150g/L、より好ましくは45~120g/Lの範囲のウォッシュコート担持量を有する、請求項1から10のいずれか1項に記載の触媒化微粒子フィルタ。
- 前記副次的な機能性材料層が、1~15g/L、好ましくは1.5~12g/L、より好ましくは2~10g/Lの範囲の担持量を有する、請求項1から11のいずれか1項に記載の触媒化微粒子フィルタ。
- 前記副次的な機能性材料層が微粒子の形態で担持される、好ましくは気相担体を介して微粒子の形態で担持される、請求項1から12のいずれか1項に記載の触媒化微粒子フィルタ。
- 前記第2の機能性材料組成物の微粒子が、1~50μm、好ましくは2~25μmのD90、及びより好ましくは3~20μmのD90を有する、請求項13に記載の触媒化微粒子フィルタ。
- (1) 請求項1から14のいずれか1項に記載の微粒子フィルタを提供する工程と、
(2) 前記エンジンからの前記排気ガスを前記微粒子フィルタに通す工程と
を含む、ガソリンエンジンからの排気ガスを処理するための方法。 - 前記排気ガスが、未燃焼の炭化水素、一酸化炭素、窒素酸化物、及び粒子状物質を含む、請求項15に記載の方法。
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