JP2007501353A - Scr濾過器を用いた排気処理システムおよび方法 - Google Patents
Scr濾過器を用いた排気処理システムおよび方法 Download PDFInfo
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- JP2007501353A JP2007501353A JP2006522653A JP2006522653A JP2007501353A JP 2007501353 A JP2007501353 A JP 2007501353A JP 2006522653 A JP2006522653 A JP 2006522653A JP 2006522653 A JP2006522653 A JP 2006522653A JP 2007501353 A JP2007501353 A JP 2007501353A
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Images
Classifications
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- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
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- B01J29/72—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing iron group metals, noble metals or copper
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- 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
- B01D53/9404—Removing only nitrogen compounds
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Abstract
Description
本発明は、1つの面において、NOxおよび粒状物を含有する排気流れを処理するに適した排気処理システム(emission treatment system)に関する。この排気処理システムは、酸化用触媒、アンモニアまたはアンモニア前駆体を前記排気流れに定期的に計量して入れる注入器、および壁流式モノリス(wall flow monolith)を含有する。前記注入器は前記酸化用触媒と流体伝達状態(fluid communication)にありかつ前記酸化用触媒の下流に位置する。前記壁流式モノリスは、SCR触媒組成物を含有し、前記注入器と流体伝達状態にありかつ前記注入器の下流に位置する。
(a)前記排気流れを酸化用触媒に通すことでNOの実質的な部分に酸化を受けさせてNO2を生じさせることでNO2が豊富な排気流れを生じさせ、
(b)アンモニアまたはアンモニア前駆体を前記NO2が豊富な排気流れに定期的な間隔で計量して入れた後、
(c)前記排気流れを壁流式モノリスに通すことで粒状物を濾過で除去しかつNOxの実質的な部分に還元を受けさせてN2を生じさせる、
ことを包含する。
(a)前記壁流式モノリスを前記SCR触媒組成物含有水性スラリーの中に1番目の方向から浸けることで前記SCR触媒組成物を入り口通路に付着させ、
(b)圧縮気体流れを出口通路の中に強制的に送り込みかつ前記入り口通路に真空をかけることで余分なスラリーを前記入り口通路から除去し、
(c)前記壁流式モノリスを前記水性スラリーの中に前記1番目の方向とは反対方向の2番目の方向から浸けることで前記SCR触媒組成物を前記出口通路に付着させ、
(d)圧縮気体流れを前記入り口通路の中に強制的に送り込みかつ前記出口通路に真空をかけることで余分なスラリーを前記出口通路から除去し、そして
(e)前記被覆を受けさせた壁流式モノリスに乾燥および焼成を受けさせる、
ことを包含する。
発明の詳細な説明
本発明は、ディーゼルエンジンの排気に含まれる粒状物、NOx及び他の気体状成分を同時に有効に処理する排気処理システムに関する。本排気処理システムでは、本排気システムが要求する重量および体積が有意に最小限になるように、使用する煤濾過器とSCR触媒を一体化させる。その上、本システムに使用する触媒組成物を選択することで、いろいろな温度の排気流れに含まれる汚染物を有効に減少させる。このような特徴は、ディーゼル車がいろいろな負荷および車速度(これらは前記自動車のエンジンから排出される排気の温度に有意な影響を与える)下で運転される場合に有利である。
寸法が5.66x6インチで壁厚が0.012インチで平均孔径が25ミクロンで壁間隙率が60%のコージライトセラミック製壁流式濾過器基質(商品名C611、NGK Insulators,Ltd.)を用いて、触媒で覆われた煤濾過器を生じさせた。
(1)前記基質を前記スラリーの中に1つの方向から前記基質の軸の長さ全体に沿って前記基質の溝が被覆されるに充分な深さに浸漬し、
(2)前記基質に前記被覆方向とは反対側(即ち乾燥している側)からエアナイフによる処理を受けさせ(air−knifed)、
(3)前記被覆側から真空をかけ、
(4)乾燥を93℃の空気流中で1時間そして焼成を400℃で1時間受けさせ、
(5)次に、段階(1)から(4)を反対側から繰り返した。
市販の自動化装置であるSuper Flow SF 1020(Probench)を用いて未被覆および被覆濾過器を横切る圧力降下を評価した。前記装置は、特に、圧力降下を空気流量の関数として測定するように考案された装置である。この装置を用いて得たデータから周囲条件下の圧力降下を空気流量の関数としてプロットした図を作成した。その圧力降下は空気が当該濾過器の中をどれだけ容易に流れるかの尺度である。ディーゼルエンジン用途では、エンジンが空気を動かす目的で動力を消費する必要があることから、圧力降下が低い方が望ましい。従って、空気のポンプ輸送で失われるエンジン動力量は圧力降下が大きければ大きいほど大きい。そのように動力が失われると車が利用することができるエンジン動力が低下してしまう。
触媒組成物を壁流式濾過器に付着させた時、それは理想的には前記濾過器の再生を補助すべきである。従って、好適には、前記濾過器の上に位置させたSCR触媒組成物が粒子のVOF部分および煤の酸化に触媒作用を及ぼす能力を有するようにする。そのSCR触媒がNOxおよび粒状物の質量を低くするに有効であるには、それは好適にはアンモニアを酸化させるべきでなくまたSO2を酸化させてSO3を生じさせるべきではない。ある触媒が炭素およびVOFを酸化させる能力を有するか否かを評価する1つの方法は、熱重量分析(TGA)と示差熱分析(DTA)を組み合わせて用いる方法である。TGAでサンプルの重量損失を測定する一方でDTAで標準と対比させたサンプルの熱容量変化を測定する。この実験では、触媒スラリーの一部に乾燥および焼成を受けさせておいて、潤滑油のVOF部分を模擬する目的で、それを6重量%の量の潤滑油と混合し、そして粒子の煤画分を模擬する目的で、それを14重量%の量のカーボンブラックと混合した。この混合物をTGAとDTAを組み合わせて実施する装置の中に充填した。いろいろなガス組成物をサンプルの中に通すことができるが、これらの試験では空気中で試験を実施した。前記装置を既知速度で加熱することで重量損失と熱発生を温度の関数として測定した。この技術の利点は、いろいろな煤成分の重量損失を分離することができかつそれらの重量損失を熱変化に関係付けることができる点にある。煤の燃焼に有効な触媒は煤の燃焼が始まる温度を低くするであろう。
ディーゼル技術の最新技術の代表例の試作エンジンであるV6で4Lのターボチャージ付き後冷却(after−cooled)ディーゼルエンジンを用いて、濾過効率と同時にNOx還元を測定した。前記エンジンをテストスタンドの上に取り付けて、それを再現可能な安定した排気をもたらすような定常状態で作動させた。前記エンジンの速度および負荷を濾過器入り口温度が370℃でNOx濃度が約950ppmになるように調節した。Code of Federal Regulations、Title 40、パート86のパラグラフ1312−88に記述されている手順に従ったが、フル希釈トンネル(full dilution tunnel)の代わりにミニ希釈トンネルを用いて粒子測定値を決定した。希釈比率をCO2濃度から決定した。前記ディーゼルエンジンに関して、尿素溶液を酸化用触媒の後方であるがSCR被覆濾過器基質の前方に注入することで、NOxの除去を達成した。この実験の構造配置を図7に示す。加熱されたサンプリングラインと分析用セルが備わっているFTIR装置を用いてNOxおよびアンモニアを測定した。また、特に生ディーゼル排気の分析に適するように考案されたHoriba分析ベンチを用いてNOx、COおよびHCも測定した。
Claims (13)
- NOxおよび粒状物を含有する排気流れを処理するに適した排気処理システムであって、
a)酸化用触媒、
b)前記酸化用触媒と流体伝達状態でそれの下流に位置していてアンモニアまたはアンモニア前駆体を前記排気流れに定期的に計量して入れる注入器、および
c)前記注入器と流体伝達状態でそれの下流に位置する壁流式モノリス、
を含んで成るが、
前記壁流式モノリスは多数の縦方向に伸びる通路を有していて、前記多数の縦方向に伸びる通路は、前記通路に境界をつけそれを限定している縦方向に伸びる壁で形成されており、ここで、前記通路は、開放された入り口末端部と封鎖された出口末端部を有する入り口通路および封鎖された入り口末端部と開放された出口末端部を有する出口通路を含んで成り、ここで、
前記壁流式モノリスは前記壁に少なくとも1.3g/立方インチの濃度で染み込んでいるSCR触媒組成物を含んで成っていて前記壁流式モノリスが有する壁間隙率が少なくとも50%で平均孔径が少なくとも5ミクロンである、
排気処理システム。 - 前記SCR触媒組成物が前記壁流式モノリスの壁に染み込んでいて前記壁が有する壁間隙率が50から75%で平均孔径が5から30ミクロンである請求項1記載の排気処理システム。
- 前記酸化用触媒と流体伝達状態でそれの上流に位置するディーゼルエンジンも更に含んで成る請求項1記載の排気処理システム。
- NOxおよび粒状物を含有する排気流れの中の生じた排気物を処理する方法であって、
(a)前記排気流れを酸化用触媒に通すことでNOの実質的な部分に酸化を受けさせてNO2を生じさせることでNO2が豊富な排気流れを生じさせ、
(b)アンモニアまたはアンモニア前駆体を前記NO2が豊富な排気流れに定期的な間隔で計量して入れた後、
(c)前記排気流れを壁流式モノリスに通すことで粒状物を濾過で除去しかつNOxの実質的な部分に還元を受けさせてN2を生じさせる、
ことを含んで成るが、
前記壁流式モノリスは多数の縦方向に伸びる通路を有していて、前記多数の縦方向に伸びる通路は、前記通路に境界をつけそれを限定している縦方向に伸びる壁で形成されており、ここで、前記通路は、開放された入り口末端部と封鎖された出口末端部を有する入り口通路および封鎖された入り口末端部と開放された出口末端部を有する出口通路を含んで成り、ここで、
前記壁流式モノリスは前記壁に少なくとも1.3g/立方インチの濃度で染み込んでいるSCR触媒組成物を含んで成っていて前記壁流式モノリスが有する壁間隙率が少なくとも50%で平均孔径が少なくとも5ミクロンである、
方法。 - 銅および鉄成分の中の1種以上から選択される卑金属成分およびゼオライトを含んで成る請求項1または4記載のSCR触媒組成物。
- 前記ゼオライトが有するアルミナに対するシリカの比率が少なくとも約10である請求項5記載のSCR触媒組成物。
- 前記ゼオライトがベータゼオライトである請求項6記載のSCR触媒組成物。
- 白金族金属成分を含んで成る請求項1または4記載の酸化用触媒。
- 更にゼオライト成分も含んで成る請求項8記載の酸化用触媒。
- 前記酸化用触媒と流体伝達状態でそれの上流に位置するディーゼルエンジンも更に含んで成る請求項4記載の方法。
- ハニカムフロースルー式モノリス基質または開放気泡発泡体基質の上に位置する請求項1または4記載の酸化用触媒。
- SCR触媒組成物を壁流式モノリスの上に位置させる方法であって、前記壁流式モノリスは、多数の縦方向に伸びる通路を有していて、前記多数の縦方向に伸びる通路は、前記通路に境界をつけそれを限定している縦方向に伸びる壁で形成されており、ここで、前記通路は、開放された入り口末端部と封鎖された出口末端部を有する入り口通路および封鎖された入り口末端部と開放された出口末端部を有する出口通路を含んで成り、
(a)前記壁流式モノリスを前記SCR触媒組成物含有水性スラリーの中に1番目の方向から浸けることで前記SCR触媒組成物を前記入り口通路に付着させ、
(b)圧縮気体流れを前記出口通路の中に強制的に送り込みかつ前記入り口通路に真空をかけることで余分なスラリーを前記入り口通路から除去し、
(c)前記壁流式モノリスを前記水性スラリーの中に前記1番目の方向とは反対方向の2番目の方向から浸けることで前記SCR触媒組成物を前記出口通路に付着させ、
(d)圧縮気体流れを前記入り口通路の中に強制的に送り込みかつ前記出口通路に真空をかけることで余分なスラリーを前記出口通路から除去し、そして
(e)前記被覆を受けさせた壁流式モノリスに乾燥および焼成を受けさせる、
ことを含んで成る方法。 - 前記壁流式モノリスが有する間隙率が少なくとも50%で平均孔径が少なくとも5ミクロンである請求項12記載の方法。
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