JP5717654B2 - ポジティブ点火エンジンから排出される排ガスから微粒子状物質を集塵するためのフィルタ - Google Patents
ポジティブ点火エンジンから排出される排ガスから微粒子状物質を集塵するためのフィルタ Download PDFInfo
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- JP5717654B2 JP5717654B2 JP2011551532A JP2011551532A JP5717654B2 JP 5717654 B2 JP5717654 B2 JP 5717654B2 JP 2011551532 A JP2011551532 A JP 2011551532A JP 2011551532 A JP2011551532 A JP 2011551532A JP 5717654 B2 JP5717654 B2 JP 5717654B2
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Images
Classifications
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Description
(i)PM−10:10μm未満の空気動力学的直径の粒子
(ii)2.5μm(PM−2.5)以下の直径を有する微細粒子
(iii)0.1μm(または100nm)以下の直径を有する超微細粒子
(iv)50nm未満の直径で特徴付けられるナノ粒子
前記多孔性基材は、焼結金属のような金属、または例えば、炭化ケイ素のようなセラミック、コーディエライト、窒化アルミニウム、窒化ケイ素、チタン酸アルミニウム、アルミナ、コーディエライト、ムライト(mullite)、例えば、針状ムライト(例えば、WO 01/16050参照)、ポルサイト(pollucite)、Al2O3ZFe、Al2O3/Ni 又は B4CZFeのようなサーメット(thermet)、またはこれらのうちのいずれか2個以上のセグメントを含む合成物になり得る。好ましい実施形態において、前記フィルタは、多数の入口チャネルと多数の出口チャネルを備えるセラミック多孔性フィルタ基材を備えるウォールフローフィルタであり、ここで、各入口チャネルおよび各出口チャネルは、多孔性構造のセラミック壁によって部分的に形成され、各入口チャネルは、多孔性構造のセラミック壁によって出口チャネルから分離される。また、前記フィルタ装置は、SAE 810114に開示されており、付加の詳細は前記書類を参照することができる。代案的に、前記フィルタは、フォーム(foam)、またはEP 1057519、もしくはWO 01/080978に記載のような、いわゆる部分フィルタ(partial filter)になり得る。
空隙は、ある間隙、微細ポア、トンネル形状(シリンダー型、プリズム型、コラム型)、スリットなどを含むことができ、前記フィルタ基材上のコーティング用ウォッシュコート合成物でコーティングされたフィルタ基材の焼成の間に燃焼される材料、例えば、分解または燃焼時にガス形成によって製造されるポアを促進させるための細断綿布(chopped cotton)または切断材料である材料を含むことにより、前記空隙が形成されることができる。空隙が存在する所で、空隙は互いに異なり、したがって、多孔性ウォッシュコートの平均粒子間ポアサイズの決定に対して考慮すべきである。
これら3つの反応は、前記TWCが化学量論的な点でまたはその周囲で駆動されるエンジンから排ガスを受け入れるときに最も効果的に作用する。本技術分野でよく公知されたように、ガソリン燃料がポジティブ点火(すなわち、スパーク点火)、内燃機関で燃焼されるときに排出される一酸化炭素(CO)、未燃焼炭化水素(HC)、および窒素酸化物(NOx)の量は、燃焼シリンダーで空気燃料混合比によって主に影響を受ける。化学量論的に均衡の取れた組成を有した排ガスは、酸化ガス(NOxおよびO2)と還元ガス(HCおよびCO)の濃度が実質的にマッチされているものである。前記化学量論的に均衡の取れた排ガス組成を発生させる空気燃料混合比(空燃比)は、通常14.7:1に与えられる。
ここで、ラムダ値1は、化学量論的に均衡の取れた(または化学量論的な)排ガス組成を表し、また、1より大きい(>1)ラムダ値は、O2およびNOxの超過を表し、その組成は「リーン(lean)」と表示され、<1より大きい(>1)ラムダ値は、HCとCOの超過を表し、その組成は「リーチ(rich)」と表示される。また、前記エンジンが作動するとき、空気燃料混合比を前記空気燃料混合比が発生する排ガス組成によって「化学量論的に」「リーン」または「リーチ」に、すなわち、化学量論的に作動されるガソリンエンジンまたはリーン−バーンガソリンエンジンとして言及するのは、本技術分野において通常的である。
したがって、挑戦は、できるだけ化学量論的な組成に近いところで前記TWC内に流入される排ガスの組成を維持するのである。
(式2)において、一酸化窒素は、NO2を形成するために、プラチナ上の活性酸化のところで酸素と反応する。(式3)は、無機硝酸塩形態にある貯蔵物質による前記NO2の吸着を含む。
(他の反応は、NH3+NOx−>N2+yH2Oまたは2NH3+2O2+CO −>N2+3H2O+CO2等に続いて、Ba(NO3)2+8H2−>BaO+2NH3+5H2Oを含む)。
金属化されるものにおいて、前記金属は、Cr、Co、Cu、Fe、Hf、La、Ce、In、V、Mn、Ni、Zn、Ga、および貴金属であるAg、Au、Pt、Pd、およびRhで構成されたグループから選択されることができる。このような金属化されたモレキュラーシーブは、還元剤を使用するポジティブ点火排ガスで窒素酸化物の還元を選択的に促進するためのプロセスに使用されることができる。ここで、「金属化」という意味は、前記モレキュラーシーブのフレームワーク(framework)内に合体される1つ以上の金属、例えば、Betaのフレームワーク内へのFe、CHAのフレームワーク内へのCuを含むモレキュラーシーブを含むものである。上述したように、前記還元剤が炭化水素である場合、前記プロセスは、時として「炭化水素の選択的な触媒還元(HC−SCR)」、「リーンNOx触媒作用」、または「DeNOx触媒作用」と呼ばれ、本出願の特定金属は、Cu、Pt、Mn、Fe、Co、Ni、Zn、Ag、Ce、およびGaを含む。炭化水素還元剤は、エンジン維持技術、例えば、後期のポスト噴射(late post injection)または初期のポスト噴射(early post injection) (「アフターインジェクション(after injection)」と呼ばれる)によって排ガス内に導入されることができる。
2個の三元触媒(TWC)コーティングが2.4g/in3のウォッシュコート荷重と85g/ft3(Pd:Rh 16:1)の貴金属荷重で準備された。1つは、ウォールフローフィルタのポア構造内(「イン−ウォール(in−wall)」)に通過するものと予測される小さい粒子サイズ(d90<5μm)で粉砕されており、他の1つは、ウォールフローフィルタ壁(「オン−ウォール(on−wall)」)の表面により近接するように位置することが優勢に予測され得るように、より少なく粉砕(d90<17μm)された。前記コーティングは、20マイクロメータ(以後では、「ミクロン」と呼ぶ)の公称平均ポアサイズ(62%の多孔率)を有し、1000分の12インチの壁厚さ(「300/12」)を有するコーディエライト製ウォールフローフィルタ基材の平方インチ当たり4.66×4.5インチの300セルに適用された。各フィルタは、水熱オーブンで約4時間の間、980℃で置かれた後、1.4L直接噴射ガソリンエンジンを有するEuro5乗客用車両上の近接連結位置に設置されている。各フィルタは、基準触媒に対する粒子数排出の減少を測定する少なくとも3個のMVEG−B駆動サイクル上で評価され、前記フィルタは、前記ウォッシュコートおよび貴金属荷重でTWCがコーティングされたフロースルー基材単一体に交替され、前記フィルタ(または基準触媒)の上流および下流に装着されたセンサの間で背圧差が決定された。
平方インチ当たり300セルのセル密度を有し、または、1000分の12インチ(ほぼ0.3mm)の壁厚さを有する5.66×3インチのコーディエライトウォールフローフィルタ基材が0.8g/in3のウォッシュコート荷重と80g/ft3のパラジウム荷重で三元触媒(TWC)コーティングでコーティングされた。次のような3つの多孔性構造が比較された:65%多孔率で38ミクロンの公称平均ポアサイズ、62%多孔率で20ミクロンの公称平均ポアサイズ、および52%多孔率で15ミクロンの公称平均ポアサイズ。各フィルタは、水熱オーブンで約4時間の間、980℃で置かれた後、1.4L直接噴射ガソリンエンジンを有し、また、近接連結された位置、すなわち、フィルタの下流に位置する完全に正式化された三元触媒でコーティングされたフロースルー基材単一体を有するEuro4乗客用車両で底の下に設置された。各フィルタは、基準システムに対する粒子数排出の減少を測定する少なくとも3個のMVEG−B駆動サイクル上で評価され、前記底の下のフィルタは、前記同一のウォッシュコート荷重およびパラジウム荷重でTWCでコーティングされたフロースルー基材単一体に交替され、前記近接するように連結されたTWCの上流に装着されたセンサと前記フィルタ(または基準触媒)の下流に装着されたセンサとの間で背圧差が決定された。
20ミクロンの公称平均ポアサイズと62%の多孔率を有する4.66×4.5インチの300/12のコーディエライトウォールフローフィルタ基材が各々0.8、1.6および2.4g/in3のウォッシュコート荷重で三元触媒コーティングでコーティングされた。各サンプルは、85g/ft3(Pd:Rh 16:1)の貴金属荷重を有した。各フィルタは、水熱オーブンで約4時間の間、980℃で置かれた後、1.4L直接噴射ガソリンエンジンを有するEuro4乗客用車両の近接連結された位置に設置された。各フィルタは、基準触媒に対する粒子数排出の減少を測定する少なくとも3個のMVEG−B駆動サイクル上で評価され、前記近接するように連結されたフィルタは、同一のウォッシュコート荷重および貴金属荷重でTWCがコーティングされたフロースルー基材単一体に交替され、ガスHC、COおよびNOx排出に対する背圧差と変換効率が前記フィルタ(または基準触媒)の上流および下流に装着されたセンサの間で決定された。単に、非メタン炭化水素(NMHC)変換が表3に報告される(Euro6に対するNMHCは、100mg/kmの全体炭化水素排出限界内で68mg/kmである)。
平方インチ当たり300セルのセル密度を有し、約0.3mmの壁厚さを有する4.66×4.5インチの300/12のコーディエライトウォールフローフィルタ基材が1.6g/in3のウォッシュコート荷重および85g/ft3(Pd:Rh 16:1)の貴金属荷重で三元触媒コーティングでコーティングされた。次のような2個の多孔性構造が比較された:65%多孔率で38ミクロンの公称平均ポアサイズ、62%多孔率で20ミクロンの公称平均ポアサイズ。より小さいポアのサンプルは評価されなかった。なぜなら、実施例2から得られた結果から、このテストで前記背圧は、Euro4乗客用車両に対してあまりにも大きくなるものと予測された。各フィルタは、水熱オーブンで約4時間の間、980℃で置かれた後、1.4L直接噴射ガソリンエンジンを有するEuro4乗客用車両で近接するように連結設置された。各フィルタは、基準触媒に対する粒子数排出の減少を測定する少なくとも3個のMVEG−B駆動サイクル上で評価され、前記近接するように連結されたフィルタは、前記同一のウォッシュコート荷重およびパラジウム荷重でTWCでコーティングされたフロースルー基材単一体に交替され、ガスHC、COおよびNOx排出に対する背圧差と変換効率が前記フィルタ(または基準触媒)の上流および下流に装着されたセンサの間で決定された。単に、非メタン炭化水素(NMHC)変換が表4に報告される。
平方インチ当たり300セルのセル密度を有し、約0.3mmの壁厚さを有する4.66×4.5インチの300/12のコーディエライトウォールフローフィルタ基材が2.4g/in3のウォッシュコート荷重および85g/ft3(Pd:Rh 16:1)の貴金属荷重で三元触媒コーティングでコーティングされた。次のような2個の多孔性構造が比較された:65%多孔率で38ミクロンの公称平均ポアサイズ、62%多孔率で20ミクロンの公称平均ポアサイズより小さいポアのサンプルは評価されなかった。なぜなら、実施例2から得られた結果から、このテストで前記背圧は、Euro5乗客用車両に対してあまりにも大きくなるものと予測された。各フィルタは、水熱オーブンで約4時間の間、980℃で置かれた後、1.4L直接噴射ガソリンエンジンを有するEuro5乗客用車両で近接するように連結設置された。各フィルタは、基準触媒に対する粒子数排出の減少を測定する少なくとも3個のMVEG−B駆動サイクル上で評価され、前記近接するように連結されたフィルタは、前記同一のウォッシュコート荷重および貴金属荷重でTWCでコーティングされたフロースルー基材単一体に交替され、前記近接するように連結されたフィルタは、同一のウォッシュコート荷重および貴金属荷重でTWCがコーティングされたフロースルー基材単一体に交替され、ガスHC、COおよびNOx排出に対する背圧差と変換効率が前記フィルタ(または基準触媒)の上流および下流に装着されたセンサの間で決定された。単に、非メタン炭化水素(NMHC)変換が表5に報告される。
13ミクロンの公称平均ポアサイズと48%の多孔率を有する1000分の5インチのセル壁厚さ(360/5)を有する118×60mmの平方インチ当たり360セルのコーディエライトウォールフローフィルタ基材が0.4および0.8g/in3のウォッシュコート荷重で三元触媒コーティングでコーティングされた。各サンプルは、85g/ft3(Pd:Rh 16:1)の貴金属荷重を有した。より大きいウォッシュコート荷重は評価されなかった。なぜなら、前記発生する背圧は、このテストでEuro4乗客用車両に対してあまりにも大きくなるものと予測されたためである。新しい(すなわち、経過していない)フィルタが1.4直接噴射ガソリンエンジンを有するEuro4乗客用車両の近接するように連結された位置に設置された。各フィルタは、基準触媒に対する粒子数排出の減少を測定する少なくとも3個のMVEG−B駆動サイクル上で評価され、前記近接するように連結されたフィルタは、前記同一のウォッシュコート荷重および貴金属荷重でTWCでコーティングされたフロースルー基材単一体に交替され、ガスHC、COおよびNOx排出に対する背圧差と変換効率が前記フィルタ(または基準触媒)の上流および下流に装着されたセンサの間で決定された。単に、非メタン炭化水素(NMHC)変換が表6に報告される。
完全に正式化された三元触媒でコーティングされた近接するように連結された位置のフロースルー基材単一体を備える2.0L直接噴射ガソリンエンジンが搭載されたEuro5乗客用車両は、MVEG−BおよびFTP(Federal Test Procedure)75駆動サイクル上でテストされた。前記MVEG−B駆動サイクルから排出される粒子の数は、PMP方法論にしたがって測定された。FTP75駆動サイクルに排出される微粒子状物質(PM)の質量は、次の基準プロトコルで測定された。0.8g/in3のウォッシュコート荷重および20g/ft3(Pd:Rh 3:1)の貴金属荷重で三元触媒コーティングでコーティングされる12ミクロンの公称平均ポアサイズと55%の多孔率を有する125×120mm、300/12のコーディエライウォールフローフィルタが底下位置、すなわち、前記フロースルー基材の単一体の下流に装着された。粒子質量と排出数の測定は繰り返された。
Claims (11)
- ポジティブ点火エンジンから排出される排ガスから微粒子状物質(PM)を集塵するためのフィルタであって、
前記フィルタが、入口面と出口面を有する多孔性基材を備え、
前記入口面が、第1平均ポアサイズのポアを備える多孔性構造によって前記出口面から分離され、
前記多孔性基材の、前記入口面か、または前記入口面および前記出口面の両方は、多孔性構造の表面ポアを実質的に覆い多数の固相粒子を含む触媒で表面がウォッシュコートでコーティングされたウォッシュコート層を備え、
前記ウォッシュコートの固相粒子のD90が、10〜40μmの範囲であり、
前記ウォッシュコートでコーティングされた多孔性基材の多孔性構造が、第2平均ポアサイズのポア(多孔)を備え、
前記ウォッシュコートでコーティングされた多孔性基材のポアが、前記ウォッシュコート内の粒子間の間隔(粒子間ポア)によって部分的に画定され、
前記第2平均ポアサイズが、前記第1平均ポアサイズ未満であり、
前記ウォッシュコートが、高い表面積の酸化物上で支持される活性成分としてのプラチナおよびロジウム、パラジウムおよびロジウム、またはプラチナ、パラジウムおよびロジウムと、酸素貯蔵成分とを含む三元触媒によるウォッシュコートである、フィルタ。 - 前記多孔性基材の多孔性構造の第1平均ポアサイズが、8〜45μmである、請求項1に記載のフィルタ。
- 前記ウォッシュコートの荷重が、0.50g in−3より大きいものである、請求項1又は2に記載のフィルタ。
- 前記ウォッシュコートの平均粒子間ポアサイズが、5.0nmないし5.0μmである、請求項1〜3の何れか一項に記載のフィルタ。
- 前記ウォッシュコートの固相粒子の平均サイズが、1〜20μmの範囲である、請求項4に記載のフィルタ。
- 前記入口面および出口面の両方がウォッシュコートでコーティングされ、
前記入口面上のウォッシュコートの平均ポアサイズが、出口面上のウォッシュコートの平均ポアサイズとは異なる、請求項1〜5の何れか一項に記載のフィルタ。 - 前記多孔性基材が、セラミックウォールフローフィルタ、金属フィルタ、またはセラミックフォームである、請求項1〜6の何れか一項に記載のフィルタ。
- 前記ウォッシュコートが、少なくとも1つのモレキュラーシーブを備えてなる、請求項1〜7の何れか一項に記載のフィルタ。
- 請求項1〜8の何れか一項に記載のフィルタを備えてなる、ポジティブ点火エンジン用排気システム。
- 請求項9に記載の排気システムを含む、ポジティブ点火エンジン。
- 表面集塵及び同時に
(i) 一酸化炭素(CO)を二酸化炭素に酸化すること;
(ii) 未燃焼炭化水素(HC)を二酸化炭素と水に酸化すること;及び
(iii) 窒素酸化物(NOx)を窒素と酸素に還元すること;
によって化学量論的な点でまたはその周囲で駆動するポジティブ点火エンジンから排出される排ガスから微粒子状物質(PM)をトラップするための方法であって、
前記方法が、PM、CO、HC及びNOxを含む排ガスと、入口面および出口面を有する多孔性基材を備えるフィルタを接触させるステップを含み、
前記入口面が、第1平均ポアサイズのポアを含む多孔性構造によって前記出口面から分離され、
前記多孔性基材の、前記入口面か、または前記入口面および前記出口面の両方は、多孔性構造の表面ポアを実質的に覆い多数の固相粒子を含む触媒で表面がウォッシュコートでコーティングされたウォッシュコート層を備え、
前記ウォッシュコートの固相粒子のD90が、10〜40μmの範囲であり、
前記ウォッシュコートでコーティングされた多孔性基材の多孔性構造が、第2平均ポアサイズのポア(多孔)を備え、
前記ウォッシュコートでコーティングされた多孔性基材のポアが、前記ウォッシュコート内の粒子間の間隔(粒子間ポア)によって部分的に画定され、
前記第2平均ポアサイズが、前記第1平均ポアサイズ未満であり、
前記ウォッシュコートが、高い表面積の酸化物上で支持される活性成分としてのプラチナおよびロジウム、パラジウムおよびロジウム、またはプラチナ、パラジウムおよびロジウムと、酸素貯蔵成分とを含む三元触媒によるウォッシュコートである、方法。
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