CN1682020B - 一种压燃式发动机及处理压燃式发动机废气的方法 - Google Patents

一种压燃式发动机及处理压燃式发动机废气的方法 Download PDF

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CN1682020B
CN1682020B CN038217295A CN03821729A CN1682020B CN 1682020 B CN1682020 B CN 1682020B CN 038217295 A CN038217295 A CN 038217295A CN 03821729 A CN03821729 A CN 03821729A CN 1682020 B CN1682020 B CN 1682020B
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motor
catalyzer
carrier material
engine
oxide
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CN1682020A (zh
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P·R·菲利普斯
M·V·特维格
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Johnson Matthey PLC
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    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
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    • B01D53/9445—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC]
    • B01D53/945—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC] characterised by a specific catalyst
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
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    • F02B1/00—Engines characterised by fuel-air mixture compression
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    • 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
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    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
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    • 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
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Abstract

一种处理来自压燃式发动机的废气的方法，其中基本上所有用于燃烧的燃料在燃烧开始之前被注入燃烧室中，该方法包括使废气与包含负载钯(Pd)催化剂的催化剂接触。

Description

一种压燃式发动机及处理压燃式发动机废气的方法
本发明涉及一种处理来自压燃式发动机的废气的方法，具体而言涉及一种其中基本上所有用于燃烧的燃料在燃烧开始之前被注入燃烧室中的发动机。 
常规的柴油机比汽油机产生的气态烃(HC)和一氧化碳(CO)少，并且通过使用铂(Pt)基柴油机氧化反应催化剂(DOC)，这些组分可能满足目前的法律限定标准。柴油机氧化氮(NOx)排放目前由发动机管理，例如废气再循环(EGR)控制。但是，结果却增加了包括挥发性和可溶性有机级分(分别记作VOF和SOF)的柴油机颗粒状物质(PM)的排放。使用DOC处理VOF和SOF以满足目前对PM的法律限定标准。 
除废气后处理之外，可以用来降低压燃式发动机排放的两种方法是发动机管理和发动机设计。最近，利用一系列发动机管理技术来降低燃烧温度而研发出了新一代的压燃式发动机。这样一种技术用于在开始燃烧之前将基本上所有用于燃烧的燃料注入到燃烧室中。 
这些技术的一个优点在于，它们能够降低NOx和PM排放，而不会显著提高燃料消耗。利用这些技术的新一代发动机的一个实施方案被称作均匀装料的压燃式(Homogeneous Charge CompressionIgnition，HCCI)柴油机。HCCI柴油机的特征包括用于通过可变的配气正时、提高的涡流比、注入速率控制(多端注入)和合适的喷射构造形成外部或内部混合物的均匀燃料供给；适合于中等燃烧速率的高稀释率；通过供料稀释和低燃烧温度得到的低NOx；和通过延长混合物制备时间得到的低PM以及因此得到的均匀性。所有相关术语均相对常规直接喷射式柴油机而言。 
另一种新式压燃式发动机被称作稀释控制燃烧系统(DilutionControlled Combustion System，DCCS)，例如Toyota的无烟富燃概念。DCCS的特征包括常规的直接注入；极高的稀释率，以通过提高点火延迟、提高涡流比、改变的配气正时和注入速率控制(多端注入)将燃烧温度降低至煤烟形成阈值之下；通过非常高的供料稀释率和极低的燃烧温度得到的低NOx和PM；以及非常高的EGR率。所有相关术语均相对常规直接喷射式柴油机而言。 
相反，典型的直接喷射式轻型柴油机在空转时产生大约50ppmNOx、1000ppm CO和800ppm HC(C1)(废气温度约185℃)；在高负载下产生大约1250ppm NOx、70ppm CO和30ppm HC(C1)(废气温度约500℃(所有值发动机断开(engine out)))； 
申请人研究了包括一种新一代发动机的交通工具的排放情况并发现，除了在降低NOx和PM方面的改进外，相对于常规直接喷射式柴油机，它们可以产生高水平的CO。在开始燃烧之前将基本上所有用于燃烧的燃料注入到燃烧室中的条件下于例如约250℃以下，这种CO排放可以表征为下列废气组成：＞2000ppm CO，如＞2500-10000ppm CO，例如＞3000ppm CO、＞4000ppm CO、＞5000ppm CO、＞6000ppm CO、＞7000ppm CO、＞8000ppm CO或＞9000ppm CO。 
另外，申请人观察到，在例如约250℃之下，例如低于200℃或低于150℃，低NOx运行条件下，这种柴油机可以产生较高水平的HC，例如＞500ppm，如600-1000ppm，例如700ppm HC、800ppmHC或900ppm HC、C1未燃烧烃(HC)。 
另外，申请人相信，从柴油机燃料的不完全燃烧可以得到不饱和烃，其实例为乙烯、丙烯、芳烃和聚芳烃。基于环境和健康原因，释放某些不饱和的HC是不希望的。 
已知目前的直接喷射式柴油机在某些运行条件下，例如在作为预热策略一部分的冷启动时或急加速之后，可以产生包含＞2000ppmCO的废气。但是，申请人相信，目前的柴油机在正常驾驶条件下不排放这么高水平的CO，或者在正常运行期间，例如在最高达250℃的温度下不排放与这么高水平的HC结合的这么高水平的CO。 
在申请人的EP 0341832中公开了一种在二氧化氮(NO2)中在最高400℃燃烧沉积在过滤器上的柴油机颗粒的方法，该NO2是通过在放置在过滤器上游的适宜催化剂上氧化废气中的一氧化氮(NO)而获得的。NO氧化反应催化剂可以包括铂族金属(PGM)，例如Pt、钯(Pd)、钌(Ru)、铑(Rh)或其组合，特别是Pt。过滤器可以涂覆上促进更高温度燃烧的材料，例如贱金属(base metal)催化剂，例如氧化钒、La/Cs/V2O5或贵金属催化剂。这种体系由Johnson Matthey以 出售。 
现在申请人已经确定了一类催化剂，它们在转化由新一代压燃式 发动机产生的废气中的较高水平的CO方面是特别有效的，特别是在温度低于约250℃时。申请人的研究还显示，这些催化剂在处理包括较高水平CO的废气中的某些HC时，比Pt DOC单独更为有效，例如在低于约250℃的温度下。实际上，申请人已经发现，在包含Pt和Pd两者的系统中处理HC，包括不饱和HC存在协同作用的迹象。 
根据一方面，本发明提供用于处理来自压燃式发动机的废气的方法，其中基本上所有用于燃烧的燃料在燃烧开始之前被注入燃烧室中，该方法包括使废气与包含负载钯(Pd)催化剂的催化剂接触。 
本文中“金属”是指在废气成分存在下存在的氧化形式的化合物，虽然在应用中它们可以以硝酸盐、碳酸盐或氢氧化物存在。 
在一个实施方案中，催化剂包括至少一种贱金属促进剂。 
在另一个实施方案中，废气包含＞2000ppm的CO。 
在另一个实施方案中，废气包含＞500ppm的C1未燃烧烃(HC)并且任选低于250℃。 
在另一个实施方案中，催化剂包含Pt，并且优选设置为使废气与Pd催化剂接触并随后与Pt接触。 
在另一个实施方案中，在Pd上燃烧废气中的CO产生放热，用以加热Pt，由此促进由Pt催化的废气组分的反应，包括HC的氧化反应和PM的燃烧。 
根据另一方面，本发明提供一种压燃式发动机，其中基本上所有用于燃烧的燃料在燃烧开始之前被注入燃烧室中，该发动机包括包含负载钯(Pd)催化剂的排放系统。 
根据一个实施方案，催化剂包括至少一种贱金属促进剂。 
根据另一个实施方案，发动机产生包含＞2000ppm CO的废气。 
根据一个实施方案，发动机产生包含＞500ppm C1未燃烧烃(HC)的废气。 
根据另一个实施方案，发动机在低于约250℃的废气温度下产生包含限定量的CO和/或HC的废气。 
在一个特定的实施方案中，根据发动机产生的废气组成，在与Pd相同或不同的载体上包含Pt是有用的。Pt可以特别用于氧化不饱和的HC，并且当然可用作处理VOF和SOF的常规DOC的主要组分。因此，用于本发明的包含Pd和Pt两者的催化剂的优点在于它可 以处理更宽范围的HC。其中一个原因是由CO中Pd组分产生的放热可以将Pt组分的温度提高至其HC起燃温度(light-off temperature)之上。 
用于Pd催化剂组分的所述至少一种贱金属促进剂可以是可还原性氧化物或碱性金属(basic metal)或其中任意两种或更多种的混合物。可还原性氧化物的示例性实例为至少一种下列元素的氧化物：锰、铁、锡、铜、钴和铈，例如下列氧化物的至少一种：MnO2、Mn2O3、Fe2O3、SnO2、CuO、CoO和CeO2。可还原性氧化物可以分散在适当的载体上和/或载体本身可包括颗粒状松散可还原性氧化物(particulate bulk reducible oxide)。CeO2的一个优点在于它是相对热稳定的，但是它易于硫中毒。氧化锰不那么热稳定，但它们更能抵抗硫中毒。可以通过将氧化锰与稳定剂如锆结合成复合氧化物或混合氧化物来改进氧化锰的热稳定性。在某种程度上，通过与适当的稳定剂如锆形成复合氧化物或混合氧化物，可以制备更耐硫的二氧化铈。 
本文中“可还原性氧化物”是指金属具有多于一种氧化态时原位存在的氧化物。在制造中，金属可以作为非氧化物化合物引入并通过煅烧被氧化为可还原性氧化物。 
碱性金属可以是碱金属，例如钾、钠或铯，碱土金属，例如钡、镁、钙或锶，或镧系金属，例如铈、镨或镧，或其中任意两种或更多种的混合物、复合氧化物或混合氧化物。在包含两种或更多种碱性金属促进剂的系统中，希望防止碱性金属之间的相互作用。因此，优选碱性金属促进剂的含量不超过Pd催化剂的3wt％。 
在一个实施方案中，碱性金属为二氧化铈，并且Pd负载在颗粒状二氧化铈上，即颗粒状二氧化铈用作Pd载体和促进剂。 
或者，PGM或每个PGM的载体可以是任何本领域已知的常规载体，例如氧化铝、氧化镁、二氧化硅-氧化铝、二氧化钛、氧化锆、沸石或其中任意两种或更多种的混合物、复合氧化物或混合氧化物，并且按照本领域的惯例，可以与碱性金属掺混。碱性金属掺杂剂的非限定性实例为锆、镧、氧化铝、钇、镨、铈、钡和钕。载体可以是例如镧稳定化的氧化铝，或包括二氧化铈和氧化锆的复合氧化物或混合氧化物，任选重量比为5∶95-95∶5。 
本文所定义的“复合氧化物”是指主要为无定形的氧化物材料， 包括至少两种元素的氧化物，它们不是由该至少两种元素组成的真正的混合氧化物。 
用于本发明的适宜的混合氧化物和复合氧化物可以通过常规方法，即共沉淀方法制备。例如，金属的可溶性盐溶液可以以适当的浓度和量混合以得到需要的终产品，然后同时使其沉淀，例如通过加入碱，如氢氧化铵。或者，已经发现利用通常已知的技术，如溶胶/凝胶或凝胶沉淀的其它制备路线也是适合的。可以将以浆料沉淀的氧化物过滤，洗涤以除去残留离子，干燥，然后在高温(＞450℃)下于空气中燃烧或煅烧。 
可如下所述制备85Mn∶15Zr复合氧化物材料。将硝酸锰(121.76g，0.425mol)和硝酸铝(28.14g，0.075mol)溶解在软化水中得到400ml溶液。小心地在2分钟内将该溶液加入到顶式搅拌的氨水溶液(150ml，2.25mol稀释至500ml)中。搅拌沉淀的浆料5分钟，然后让其“老化”30分钟。过滤回收沉淀物并洗涤直到滤液的电导率为1500μScm-1。在100℃使该材料干燥，然后在350℃燃烧2小时(以10℃/min升温和降温)。 
以催化剂的总重量为基准，催化剂可包含0.1-30wt％，任选0.5-15wt％且优选1-5wt％的PGM。在一个实施方案中，催化剂包含重量比为100∶0-10∶90的Pd∶Pt。在另一个实施方案中，催化剂包含占催化剂总重量0.1-10wt％的Pt和占催化剂总重量0.1-20wt％的Pd。根据另一个实施方案，排放系统包含30-300gft-3的Pd和30-300gft-3的Pt(如果存在)。 
催化转换器可包括常规的底物，例如陶瓷如堇青石，或金属如FecralloyTM，蜂窝状整料(monolith)。在一个特定的实施方案中，一种或两种底物包括微粒过滤器，例如陶瓷壁流过滤器，例如上游的底物可以是流经性底物，而下游的底物是过滤器。如果需要，催化剂可以涂覆在过滤器的下游端部。当单独存在的铂族金属(PGM)是Pd时，单一底物上可涂覆有活性催化剂涂层(washcoat layer)，该层包含负载的Pd和所述至少一种贱金属促进剂。但是，当催化剂也包含Pt时，申请人认为催化转换器可以采取几种方式中的一种。 
在一个实施方案中，Pd和Pt均负载在相同的颗粒状载体材料上。 
在另一个包含单一底物的实施方案中，负载Pd和所述至少一种 贱金属促进剂涂覆在底物的上游部分，而Pt涂覆在其下游部分，虽然如果需要，Pt也可以在Pd的上游。 
在一个也包含单一底物的可替换实施方案中，Pt放置在底物上的第一层中，而负载Pd和所述至少一种贱金属促进剂放置在覆盖第一层上的第二层中。但是，如果需要，Pd可以位于上层，而Pt位于下层。 
在也包含单一底物的第四种实施方案中，底物涂覆有一层活性催化剂涂层，其中第一颗粒状载体包括负载Pd和所述至少一种贱金属促进剂，并且Pt负载在第二颗粒状载体上，其中第一和第二载体放置在单层底物上。 
在一个可替换的实施方案中，排放系统包括包含负载Pd和所述至少一种贱金属促进剂的第一底物和包含Pt的第二底物，该第二底物放置在第一底物的下游。如果需要，第一底物和第二底物的顺序可以颠倒。 
在新一代安装了柴油机的交通工具中，可以控制发动机以在整个发动机负荷转速图中将基本上所有用于燃烧的燃料在燃烧开始之前注入到燃烧室中的模式运行。但是，申请人认为，在特定的实施方案中，发动机控制装置可以将发动机转换为在高负载下直接喷射式柴油机所用的更常规的柴油机燃烧模式。在这种“直接喷射”运行期间，可能需要处理NOx和PM的水平，以便该交通工具整体上满足相关排放法规。 
根据一个特定的实施方案，本发明提供了根据本发明具有第一运行条件和第二条件的发动机，在第一条件中发动机被构造为在至少一部分发动机循环期间以将基本上所有用于燃烧的燃料在燃烧开始之前注入到燃烧室中的模式运行，在第二条件中发动机被构造为以常规直接喷射式柴油机模式运行。对第一和第二运行条件的控制可以通过与发动机所带的发动机控制装置来实现，例如包括预程序化的处理器，例如中央处理器(CPU)，任选形成发动机控制单元(ECU)的一部分。 
当要求额外对废气进行后处理以便在第二运行条件期间处理废气时，可以将任选催化的微粒过滤器放置在Pd催化剂和结合的所述至少一种贱金属促进剂以及如果存在的Pt催化剂的下游。这种设计 记载于申请人的EP 0341832中，其中废气中的NO被Pd催化剂氧化为NO2，而收集在过滤器上的废气中的颗粒在NO2中于最高达400℃的温度下燃烧。如果需要，Pt催化剂可以放置在过滤器上。 
当根据本发明的发动机包括废气再循环阀和回路以使所选择部分的废气再循环进入发动机空气入口，理想的是，在与发动机入口空气混合之前将废气冷却。 
根据本发明的压燃式发动机可以是柴油机，例如被相关法规所限定的诸如轻型柴油机或重型柴油机。 
其中本发明的排放系统可以有利地使用的发动机的两个实施方案为均匀装料的压燃式(HCCI)柴油机和稀释控制燃烧系统(DCCS)柴油机。 
根据另一方面，本发明提供了一种包括本发明发动机的交通工具。 
为了更充分地理解本发明，仅以例举的方式给出下列实施例。所有给出的温度指入口气体的温度。 
实施例1 
试验下列催化剂对HC和CO在模拟的催化剂活性试验(SCAT)气体成套装置(gas rig)中的起燃效果：2wt％Pt-氧化铝基催化剂(催化剂A)、2wt％Pd-氧化铝基催化剂(催化剂B)和2wt％Pd-二氧化铈基催化剂(催化剂C)。对每种催化剂样品在表1所列的流动气体混合物中进行试验。所用气体混合物的温度在每个试验中从100℃升高至500℃。 
表1：用于进行催化剂A、B和C活性试验的气体混合物 
   气体混合物1  气体混合物2  气体混合物3  气体混合物4
  ppm HC(C1)丙烯   600   900   3000   3000
  ppm CO   200   600   25000   25000
  ppm NO   200   200   200   200
  ％H2O   4.5   4.5   4.5   4.5
  ％O2   12   12   12   3
  ％CO2   4.5   4.5   4.5   4.5
  ppm SO2   20   20   20   20
  N2   余量   余量   余量   余量
  流速  (升/小时/g样品)   300   300   300   300
  升温速度  (℃/min)   10   10   10   10
气体混合物1和2具有与来自常规运行的柴油机的典型废气相同的HC和CO气体浓度。气体混合物3具有比气体混合物1和2更高的HC和CO浓度，而气体混合物4具有比气体混合物1-3所用的更低的氧浓度。表2和3显示了在每种催化剂上达到80％HC和CO氧化转化时的温度。 
表2：气体混合物1-3使用催化剂A、B和C达到80％转化(T80HC/CO)时的温度 
  T80 HC/CO(℃)   气体混合物1   气体混合物2   气体混合物3
  催化剂A   170/＜110   158/114   185/183
  催化剂B   264/265   253/247   205/203
  催化剂C   231/164   226/170   ＜110/＜110
在较低温度使用气体混合物1和2进行HC和CO氧化反应时，催化剂A显示出比催化剂B或C明显更高的活性，但在高HC和CO气体混合物3中显示出低温氧化活性的损失。与催化剂A在高HC和 CO气体进料中活性损失相反，从气体混合物1或2至气体混合物3，催化剂B在低温氧化活性方面显示出小的改进。但是，尽管催化剂B对较高HC和CO气体进料条件的低温氧化活性有改进，但催化剂B的总体活性比催化剂A的差。相反，相对于催化剂A，催化剂C对于气体混合物1和2下显示出更低的活性。但是，与催化剂A和催化剂B相反，对于高HC和CO浓度的气体混合物3的低温HC和CO氧化，催化剂C显示出最高的活性。 
表3显示，与在包含12％氧的气体混合物3中测定的活性相比，催化剂A的低温CO活性在包含3％氧的气体混合物4中进一步降低。相反，与气体混合物3相比，催化剂B在气体混合物4中的活性稍有改进。在气体混合物3和4中催化剂C的低温氧化活性均保持非常高。这些数据显示，在CO存在下，Pd比Pt活性更高。 
表3：气体混合物3和4使用催化剂A、B和C达到80％转化(T80-CO)时的温度 
  T80 CO(℃)   混合物3   混合物4
  催化剂A   183   239
  催化剂B   203   197
  催化剂C   ＜110   ＜110
实施例2 
在另一系列的活性试验中，使用表4所列的气体混合物测试催化剂D(1wt％ Pt-氧化铝基)和催化剂E(4wt％Pd-二氧化铈基)对HC和CO在SCAT气体成套装置(gas rig)中的起燃效果，通过每种样品的气体的温度在每个试验期间从100℃升高至500℃。 
表4：用于进行催化剂D和E活性试验的气体混合物 
    气体混合  物5   气体混合  物6   气体混合  物7   气体混合  物8   气体混合  物9
  ppm HC(C1)甲苯   600   600   600   600   600
  ppm CO   200   950   2000   10000   25000
  ppm NO   200   200   200   200   200
  ％H2O   4.5   4.5   4.5   4.5   4.5
  ％O2   12   12   12   12   12
  ％CO2   4.5   4.5   4.5   4.5   4.5
  ppm SO2   20   20   20   20   20
  N2   余量   余量   余量   余量   余量
  流速  (升/小时/g  样品)   300   300   300   300   300
  升温速度  (℃/min)   10   10   10   10   10
对于从5至9的气体混合物，CO浓度都渐进地提高，并且其余气体用余量氮气保持恒定。表5显示了CO浓度对催化剂的HC和CO起燃的影响。 
表5：气体混合物5-9使用催化剂D和E达到80％转化(T80-HC/CO)时的温度 
  T80 HC/CO  (℃)   气体混合物5   气体混合物6   气体混合物7   气体混合物8   气体混合物9
  催化剂D   188/112   192/158   194/185   212/210   231/217
  催化剂E   259/135   256/130   175/＜110   ＜110/＜110   ＜110/＜110
催化剂D显示，随着CO浓度渐进提高，其低温活性损失，而催化剂E则显示在更高CO的气体进料下低温活性有改进。申请人推断，催化剂D的活性损失是由于催化剂上的活化点的自身中毒。众所周 知，在Pt活化点上CO的强烈吸附可能阻止形成CO2的氧化反应所必需的氧的吸附。催化剂E不显示这种自身中毒行为，该催化剂在较高CO浓度下氧化CO的活性明显高于催化剂A和D。 
实施例3 
使用含有25000ppm CO和两种不同HC浓度(使用丙烯或甲苯)的气体混合物进一步进行催化剂D(1wt％Pt-氧化铝基)和催化剂E(4wt％Pd-二氧化铈基)在SCAT成套装置中的试验。将每种催化剂样品放在表6所示的气体混合物中，气体的温度从100℃升高至500℃。使用丙烯或甲苯作为HC物质使HC(C1)的浓度由600ppm提高到3000ppm。所测试的催化剂活性示于表7中。 
表6：用于进行催化剂A和催化剂C活性试验的气体混合物 
    气体混合物  10   气体混合物  11   气体混合物  12   气体混合物  13
  ppm HC(C1)丙烯   600   3000   0   0
  ppm HC(C1)甲苯   0   0   600   3000
  ppm CO   25000   25000   25000   25000
  ppm NO   200   200   200   200
  ％H2O   4.5   4.5   4.5   4.5
  ％O2   12   12   12   12
  ％CO2   4.5   4.5   4.5   4.5
  ppm SO2   20   20   20   20
  N2   余量   余量   余量   余量
  流速  (升/小时/g样品)   300   300   300   300
  升温速度  (℃/min)   10   10   10   10
表7：气体混合物10-13中使用催化剂D和E达到80％转化(T80-CO/HC)时的温度 
  T80 HC/CO(℃)   气体混合物  10   气体混合物  11   气体混合物  12   气体混合物  13
  催化剂D   186/184   218/218   231/217   230/231
  催化剂E   ＜110/＜110   ＜110/＜110   ＜110/＜110   ＜110/＜110
对于气体混合物10和12(包含25000ppm CO、600ppm HC)，催化剂E显示了最高的HC和CO起燃活性。相对于气体混合物10或12中发现的活性，催化剂D在气体混合物11和13(包含25000ppmCO、3000ppm HC)中的起燃活性恶化。催化剂E在所有使用的气体混合物中的活性均比催化剂D的高。 
实施例4 
使用含有10000ppm CO和四种不同HC浓度(使用丙烯)的气体混合物进一步进行催化剂A、B和C在SCAT成套装置中的试验。将每种催化剂样品在表8所示的气体混合物中试验，气体的温度从100℃升高至500℃。HC(C1)的浓度由600ppm提高到4500ppm(丙烯)。催化剂的活性示于表9中。 
表8：用于进行催化剂A、B和催化剂C活性试验的气体混合物 
    气体混合物  14   气体混合物  15   气体混合物  16   气体混合物  17
  ppm HC(C1)丙烯   600   1800   3000   4500
  ppm CO   10000   10000   10000   10000
  ppm NO   200   200   200   200
  ％H2O   4.5   4.5   4.5   4.5
  ％O2   12   12   12   12
  ％CO2   4.5   4.5   4.5   4.5
  ppm SO2   20   20   20   20
  N2   余量   余量   余量   余量
  流速  (升/小时/g样品)   300   300   300   300
  升温速度  (℃/min)   10   10   10   10
[0079]  表9：气体混合物14-17中使用催化剂A、B和C达到80％(T80-CO/HC)时的温度 
Figure G200380021729501D00141
催化剂C显示对包含600ppm HC的气体进料中HC和CO氧化反应的活性最高。催化剂B的活性最差。升高的HC水平引起催化剂活性的少许下降，但相对于催化剂A和B，即使是在最高的HC水平，催化剂C也具有低得多的氧化起燃低温活性。 
实施例5 
使用含有1％CO和1000ppm浓度下三种不同HC物质(C3)的气体混合物进行催化剂C(2wt％Pd-二氧化铈)、催化剂F(2.5wt％Pt-氧化铝基)和催化剂G(1.25wt％Pt/1wt％ Pd，即催化剂C和催化剂F的混合物)的另一系列的SCAT试验。试验过程如前实施例1中所述，并且气体混合物如表10所示。所测得的催化剂活性示于表11中。 
表10：用于进行催化剂C、F和G活性试验的气体混合物 
    气体混合物18   气体混合物19   气体混合物20
  ppm HC(C3)丙烯   1000   0   0
  乙烯   0   1000   0
  乙烷   0   0   1000
  ppm CO   10,000   10,000   10,000
  ppm NO   200   200   200
  ％H2O   4.5   4.5   4.5
  ％O2   12   12   12
  ％CO2   4.5   4.5   4.5
  ppm SO2   20   20   20
  N2   余量   余量   余量
  流速  (升/小时/g样品)   300   300   300
  升温速度  (℃/min)   10   10   10
表11：气体混合物18、19和20中使用催化剂C、F和G达到80％和50％转化(CO/HC)时的温度 
Figure G200380021729501D00151
虽然催化剂C对低温CO氧化保持了高效率，但催化剂F对于除丙烯之外的短链HC的氧化保持更高的效率。混合体系催化剂G显示了与催化剂C的活性不相似的良好的CO活性。催化剂G显示了与催化剂C相当的丙烯起燃以及低得多的对乙烯和乙烷的起燃，证明通过组合两种催化剂制剂可以获得强烈的协同效应。 
实施例6 
在气体混合物3(高CO和HC浓度)和气体混合物21(低CO和HC浓度)中，与催化剂A(2wt％Pd-Al2O3)和催化剂C(2wt％Pd-Ce)对比评定其它金属载体(metal support)的效果。待评价的其它催化剂是催化剂H(2wt％Pd-MnO2(Aldrich))、催化剂I(2wt％Pd-Mn：Zr[85.15])和催化剂J(2wt％Pd-20wt％Ba/Al2O3)。试验过程如前所述，并且气体混合物如表12所示，催化剂活性归纳于表13中。 
表12：用于进行催化剂A、C、H、I和J活性试验的气体混合物 
    气体混合物21   气体混合物3
  ppm HC(C1)丙烯   900   3000
  ppm CO   1000   25000
  ppm NO   200   200
  ％H2O   4.5   4.5
  ％O2   12   12
  ％CO2   4.5   4.5
  ppm SO2   20   20
  N2   余量   余量
  流速(升/小时/g样品)   300   300
  升温速度(℃/min)   10   10
[0093]  表13：气体混合物3和21中使用催化剂A、C、H、I和J达到80％和50％转化(CO/HC)时的温度 
Figure G200380021729501D00171
含锰催化剂H和I均显示了高CO浓度时与催化剂C相当的性能，但在低CO浓度时起燃更低。与低CO浓度相比，在高CO浓度时加入Ba(催化剂J)显示出改进的性能，并且与催化剂A相比，具有极好的活性。 
实施例7 
在满足欧III(European Stage 3)法规要求并且以含硫＜10ppm的柴油燃料为燃料的1.9升共用燃油油轨的直接喷射式涡轮增压柴油机车上装配直径为4.66英寸(118mm)、长为6英寸(152mm)的陶瓷负载催化剂。用铂催化剂以140gft-3(4.85gL-1)涂覆催化剂K，并且用铂催化剂以70gft-3(2.43gL-1)和用钯-二氧化铈催化剂以70gft-3(2.43gL-1)的钯负载量涂覆催化剂L。测试前，在700℃使催化剂老化5小时。 
改变发动机的废气排放以再现一定范围的废气条件。这些变化是通过改变一个或多个下列参数获得的：再循环排气率(EGR率)、预喷射正时(pilot injection timing)和喷射燃料量、主喷射正时(maininjection timing)、共用燃油油轨燃料压力和涡轮增压机的增压。随着这些标准的改变，可以提高发动机的HC和CO水平。 
两种催化剂均以具有标准生成标度(calibration)(基本标度)的欧洲III试验循环进行评价。然后用生成比基本标度高3倍的CO排放的标度进行评价。表14归纳了两种催化剂在两种标度下的结果。 
表14：催化剂A和B在两种标度下的结果(g/km) 
Figure G200380021729501D00181
从表14可见，在基本标度下，对CO的排放，各催化剂具有非常相似的性能。在高CO标度下，催化剂L具有比催化剂K低得多的尾管HC和CO排放。 
用于提高来自发动机的CO排放的方法还导致NOx的显著提高。在专门设计的在产生这些高CO排放的条件下运行的发动机类型中不会发生上述情况。但是，结果显示，两种催化剂的氧化性能均不依赖于NOx的浓度，因此，在合成气体试验中使用恒定的200ppm的NOx浓度对所获得的HC和CO氧化的结果没有影响。 

Claims (20)

1.一种柴油压燃式发动机，其包括在使用时用于控制发动机燃料燃烧模式的控制装置和排放系统，所述排放系统包括一种包含钯、铂和至少一种贱金属促进剂的催化剂，该至少一种贱金属促进剂由选自锰、铁、钴、铜、锡和铈的可还原性氧化物组成，其中所述钯负载在含有所述至少一种贱金属促进剂的第一载体材料上，并且所述铂负载在第二载体材料上，该第二载体材料选自氧化铝，用选自锆、钇、镨、钡和钕的贱金属掺混的氧化铝，氧化硅-氧化铝以及镧稳定化的氧化铝，其中所述控制装置控制发动机在至少一部分发动机循环期间将基本上所有用于燃烧的燃料在燃烧开始之前注入到燃烧室中的模式下运行。
2.根据权利要求1的发动机，其中控制装置控制发动机在一部分发动机循环期间以常规直接喷射式柴油机模式运行。
3.根据权利要求2的发动机，其中在发动机被控制以常规直接喷射式柴油机模式运行中的一部分发动机循环包括高发动机负载。
4.根据权利要求1、2或3的发动机，其中在基本上所有用于燃烧的燃料在燃烧开始之前注入到燃烧室中的模式中，发动机排放所产生的废气包含＞2000ppm的一氧化碳。
5.根据权利要求1的发动机，其中在基本上所有用于燃烧的燃料在燃烧开始之前注入到燃烧室中的模式中，发动机排放所产生的废气包含＞500ppm的C1未燃烃。
6.根据权利要求1的发动机，其中在基本上所有用于燃烧的燃料在燃烧开始之前注入到燃烧室中的模式中，发动机排放产生温度低于250℃的废气。
7.根据权利要求1的发动机，其中所述至少一种可还原性氧化物为选自MnO2、Mn2O3、Fe2O3、CuO、CoO、SnO2和CeO2的至少一种。
8.根据权利要求1的发动机，其中该可还原性氧化物分散在载体材料上。
9.根据权利要求1的发动机，其中载体本身包括颗粒状可还原性氧化物。
10.根据权利要求1的发动机，其中所述催化剂包括选自以下的方案：
(i)第一载体材料放置在第一基质整体上，而第二载体材料放置在第二基质整体上，该第二基质整体放置在第一基质整体的下游；
(ii)第一载体材料放置在基质整体的上游部分，而第二载体材料放置在该基质整体的下游部分；
(iii)第二载体材料放置在基质整体上的第一层中，而第一载体材料放置在覆盖第一层的第二层中；和
(iv)包括单层的基质整体，所述单层包括第一和第二载体材料。
11.根据权利要求1的发动机，其中第一载体材料选自氧化铝、氧化硅-氧化铝、二氧化铈、氧化镁、二氧化钛、氧化锆、沸石或其中任意两种或多种的混合物、复合氧化物或混合氧化物中的至少一种。
12.根据权利要求1的发动机，其中第二载体材料选自氧化铝、氧化硅-氧化铝，氧化铝和氧化锆的复合氧化物或混合氧化物。
13.根据权利要求1的发动机，其中催化剂包含占催化剂总重量0.1-30wt％的铂族金属。
14.根据权利要求13的发动机，其中催化剂包含占催化剂总重量0.5-15wt％的铂族金属。
15.根据权利要求14的发动机，其中催化剂包含占催化剂总重量1-5wt％的铂族金属。
16.根据权利要求1的发动机，其中该催化剂包含占催化剂总重量0.1-10wt％的Pt和占催化剂总重量0.1-20wt％的Pd。
17.根据权利要求1的发动机，其中该排放系统包括放置在负载Pd下游的任选的催化的微粒过滤器。
18.根据权利要求1的发动机，其中所述发动机是均匀装料的压燃式柴油机或稀释控制燃烧系统柴油机。
19.包括根据权利要求1-18中任意一项的发动机的交通工具。
20.一种处理来自柴油压燃式发动机的废气的方法，其中所述发动机在基本上所有用于燃烧的燃料在燃烧开始之前被注入燃烧室中的模式下操作，该方法包括使废气与包含钯、铂和至少一种贱金属促进剂的催化剂接触，该至少一种贱金属促进剂由选自锰、铁、钴、铜、锡和铈的可还原性氧化物组成，其中所述钯负载在含有贱金属促进剂的第一载体材料上，并且铂负载在第二载体材料上，该第二载体材料选自氧化铝，用选自锆、钇、镨、钡和钕的贱金属掺混的氧化铝，氧化硅-氧化铝，以及镧稳定化的氧化铝。
CN038217295A 2002-09-13 2003-09-15 一种压燃式发动机及处理压燃式发动机废气的方法 Expired - Fee Related CN1682020B (zh)

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WO2004025096A1 (en) 2004-03-25

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