CN101559325A - 还原汽油发动机废气流中的排放物的催化剂系统及其方法 - Google Patents

还原汽油发动机废气流中的排放物的催化剂系统及其方法 Download PDF

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CN101559325A
CN101559325A CNA2009101299363A CN200910129936A CN101559325A CN 101559325 A CN101559325 A CN 101559325A CN A2009101299363 A CNA2009101299363 A CN A2009101299363A CN 200910129936 A CN200910129936 A CN 200910129936A CN 101559325 A CN101559325 A CN 101559325A
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哈兰德·S·甘地
罗伯特·瓦尔特·麦卡贝
约瑟夫·罗伯特·泰斯
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Abstract

本发明公开了一种还原汽油发动机废气流中的排放物的催化剂系统及方法。描述了用于提高稀燃NOx后处理系统的耐用性的实施例。根据本发明的一个实施例，当发动机以化学计算的或富燃空气燃油比率运转并且废气温度在可校准的水平(例如700℃)以上时，空气注入系统被用于连续地将空气注入在上游三元催化剂和下游选择性催化还原(SCR)催化剂之间的排气系统。这产生整体稀燃混合物并避免将SCR催化剂暴露给热的富燃条件或热的化学计算的条件。被注入的空气还将使热的废气冷却，这也将对SCR催化剂的耐用性有利。在另一实施例中，在原地产生用于SCR的还原剂，在另一实施例中，使用用于具有还原剂的旁路臂的换向阀以在高载条件过程中绕开SCR。

Description

还原汽油发动机废气流中的排放物的催化剂系统及其方法
技术领域
本发明的一方面涉及一种在汽油发动机的稀燃过程中控制NOX排放物的选择性催化还原(SCR)系统，该系统由于增加了保护SCR催化剂以避开不利条件的空气注入系统，所以耐用性得到提高。本发明的其它方面包括使用空气注入系统以保护与其它催化剂结合的SCR催化剂以及原位系统，从而SCR在轻载条件下对于稀燃NOX转化是耐用且有效的，并且完全得到用于高载运转的其它催化剂系统的支持。
背景技术
内燃机正面临着减少有害副产品的排放的需要以及提高燃油经济性的日益增加的压力这样的挑战。由氮的氧化物组成的NOX构成了这些副产品的主要成分。
与被设计成以化学正确(chemically correct)(化学计算，stoichiometric)的大约14.7∶1的空气燃油比率运转的传统汽油发动机相比，稀燃发动机被设计成在轻载条件过程中以非常稀燃的空气燃油比率运转，14.7∶1的空气燃油比率对于三元催化剂性能是优化的。当不需要全功率时，在轻载条件过程中，稀燃发动机将过量的空气与燃油混合，使得燃油经济性更好。稀燃进气道燃油喷射汽油发动机(lean burn port-fuel-injected gasoline engine)中的空气燃油比率可高达22∶1，对于在分层进气条件下运转的直喷(DI)汽油发动机来说，空气燃油比率可高达30∶1。在重载条件过程中，例如在加速或爬坡过程中，当需要全功率时，稀燃发动机回复到化学计算的比率(14.7∶1)或更富燃的比率。
折衷解释，如果通过将空气与燃油的比率增加到稀燃条件来增加发动机效率，则降低一氧化碳和颗粒排放物。然而，用于当前化学计算的发动机的排放物控制的三元催化剂在稀燃环境中NOX转化效率不足。相反，如果将燃烧过程修改为还原氧化氮产物，即，通过在富燃(燃料过剩)的条件下使发动机运转，则颗粒、一氧化碳以及碳氢化合物排放物增加并且燃油效率显著降低。
选择性催化还原(SCR)是在稀燃条件下通过催化剂选择性地还原NOX的过程。利用还原剂(例如，尿素或NH3)的选择性催化还原是用于处理来自柴油发动机的NOX排放物的有效技术。SCR催化剂使用碱金属来促进NOX和NH3之间的反应，以在稀燃条件下产生N2和H2O。SCR催化剂可在宽的温度范围内还原NOX，并且由于它们不含有贵金属，所以它们是柴油NOX控制的节省成本的方法。SCR的一个问题是需要在车上携带额外的还原剂。由于处理NH3存在安全问题，所以这种还原剂通常是尿素。尿素在排气系统中分解成NH3，NH3与NOX通过SCR反应以形成N2。
利用尿素或NH3注入的选择性催化还原(SCR)还是用于稀燃汽油发动机(稀燃进气道燃油喷射(PFI)或分层进气DI发动机)上NOX控制的主要候选方案。然而，在高载运转过程中，汽油发动机以化学计算的或富燃A/F比率正常地运转，产生的热的富燃废气(hot rich exhaust)或热的化学计算的废气(hot stoichiometric exhaust)对SCR催化剂的耐用性有害，导致NOX转化能力降低。
因此，在高温的富燃或化学计算运转的过程中，需要保护SCR催化剂，从而当废气温度降低并且空气燃油比率回复到稀燃条件时能够保持高的NOX转化效率。
发明内容
根据本发明的一个实施例，提供了一种还原稀燃汽油发动机废气流中的有害的排放物的耐用的催化剂系统，该系统包括：点火催化剂，紧密地结合到发动机；选择性催化还原催化剂，位于点火催化剂的下游；还原剂注入系统，位于点火催化剂和选择性催化还原催化剂之间；空气注入系统，位于点火催化剂和还原剂注入的位置之间，用于将空气注入到处于预先指定的发动机条件下的废气流内，以提高选择性催化还原催化剂的耐用性。所述空气注入系统可以是在指定的条件下提供连续的空气流的泵
根据本发明的另一实施例，提供了一种用于提高还原稀燃汽油发动机的有害排放物的催化剂系统的耐用性的方法，该方法包括下述步骤：提供催化剂系统，该催化剂系统包括紧密地结合到发动机的点火催化剂以及位于点火催化剂下游的选择性催化还原催化剂；在对选择性催化还原催化剂的耐用性有害的某些指定的发动机条件下将空气注入于点火催化剂和选择性催化还原催化剂之间。
在本发明的另一实施例中，提高了一种用于提高还原汽油发动机的废气排放物中的有害排放物的催化剂系统的耐用性的方法，该方法包括下述步骤：提供催化剂系统，该催化剂系统包括紧密地结合到发动机的点火催化剂以及位于点火催化剂下游的选择性催化还原催化剂；在某些指定的发动机条件下将空气注入于点火催化剂和选择性催化还原催化剂之间；当温度在选择性催化还原催化剂的工作范围内时，在选择性催化还原催化剂的上游注入还原剂；在空气注入的位置和还原剂注入的位置之间提供氧化催化剂，以防止SCR催化剂发生放热反应并防止热分解的发生。
在本发明的另一实施例中，提供了一种还原稀燃汽油发动机废气流中的有害排放物的耐用的催化剂系统，该系统包括：点火催化剂，紧密地结合到发动机；选择性催化还原催化剂，位于点火催化剂的下游；还原剂注入系统，位于点火催化剂和选择性催化还原催化剂之间；换向阀，位于还原剂注入的位置的下游和SCR的上游，所述换向阀连接到包括三元催化剂的旁路臂，该换向阀可被用于在高载条件下绕开选择性催化还原催化剂并提高NOX转化率。
在本发明的另一实施例中，在富燃清污阶段中，通过在选择性催化还原催化剂的上游的稀燃NOX吸收装置在原地产生氨，并且空气注入系统位于稀燃NOX吸收装置和选择性催化还原催化剂之间，从而可在对选择性催化还原催化剂的耐用性有害的某些指定的发动机条件下注入空气。
考虑到本发明的下面的详细的描述，本发明的这些和其它方面将被更好地理解。
附图说明
在此描述的本发明的实施例将按照稳定的方式在权利要求书中被描述。然而，通过参照下面结合附图进行的详细的描述，其它特点将变得更加清楚并且实施例会被更好地理解，其中：
图1显示对于铁/沸石SCR催化剂的NOX转化率与温度之间的关系，以证明铁/沸石SCR在稀燃废气中比在富燃或化学计算的废气中更耐用；
图2显示对于铜/沸石SCR催化剂的NOX转化率与温度之间的关系，以证明铜/沸石SCR在稀燃或化学计算的废气中比在富燃废气中更耐用；
图3是使选择性催化还原催化剂的放热反应最小化的包括空气注入和还原剂注入以及氧化催化剂的建议的排气系统的示意图；
图4是描述具有换向阀以及含有另外的三元催化剂的旁路臂的排气系统的示意图；
图5A和图5B是描述带有空气注入以保护SCR催化剂的LNT+SCR原位系统的示意图。
具体实施方式
选择性催化还原(SCR)催化剂是在汽油发动机的稀燃操作过程中用于NOX控制的主要候选物。SCR催化剂使用碱金属来促进NOX和NH3之间的反应以在稀燃条件下产生N2。与其它现有技术相比，由于SCR催化剂可在宽的温度范围内工作，所以SCR催化剂是有利的，对送入的气(feedgas)NOX的浓度要求不高(robust)，并且因为SCR催化剂不需要使用贵金属，所以它们节省成本。然而，在高载运转过程中，汽油发动机以化学计算的或富燃空气燃油比率正常运转，产生的热的富燃废气或热的化学计算的废气对SCR催化剂的耐用性有害。在这种热的条件下，SCR催化剂必须被保护，以当废气温度降低和空气燃油比率回复到稀燃条件时保持SCR催化剂的NOX转化能力。
目前开发的用于车辆应用的SCR配方(formulation)包括铁/沸石配方和铜/沸石配方。
在本发明的一个实施例中，当发动机以化学计算的或富燃A/F比率运转并且废气温度在可校准的水平(calibratible level)(例如，700℃)之上时，通过使用注空气(air injection)或脉冲空气以将空气连续地注入到紧密地结合(close coupled)的点火催化剂(例如，三元催化剂(TWC))和SCR催化剂之间的废气内，SCR催化剂被保护以避开这种热条件。这将产生整体稀燃混合物并避免使SCR催化剂被暴露给热的富燃条件或热的化学计算的条件。注入的空气还将使热的废气冷却，这也将对SCR的耐用性有利。
为了证实SCR在稀燃废气中比在富燃或化学计算的废气中更耐用，在脉冲火焰燃烧反应堆(pulse-flame combustion reactor)上以800℃的入口温度将铁/沸石SCR催化剂的样本老化34小时。一个样本在A/F比率大部分时间是富燃的耐用性循环上被老化。另一个样本在A/F比率大部分时间是化学计算的耐用性循环上被老化。第三个SCR样本通过向废气内注入氧气而以稀燃A/F比率被持续老化。在实验室反应堆上，对这三个老化样本进行评估，其中，送入的气含有500ppm的NO和500ppm的NH3以及5％的O2、10％的CO2、10％的H2O以及平衡量的N2。熔炉的温度从150℃的熔炉温度缓慢上升到800℃以上的温度。K型热电偶用于测量SCR催化剂的床温度(bedtemperature)。
在图1中将3个样本的NOX转化率显示为测量的温度的函数。
图1示出了铁/沸石SCR催化剂在脉冲火焰燃烧反应堆上以800℃的温度针对主要为富燃老化循环、主要为化学计算的老化循环或持续稀燃老化循环老化34小时的的NOX转化率与温度的关系。在缓慢的温度上升过程中用500ppm的NO和500ppm的NH3在实验室反应堆上进行评估。
用连续的稀燃废气老化的样本比按照利用主要为化学计算的运转的进程老化的样本具有更好的性能，而按照利用主要为化学计算的运转的进程老化的样本比按照利用主要为富燃运转的进程老化的样本具有稍好的NOX转化率。这证明铁/沸石SCR催化剂的耐用性在高温稀燃废气中比在高温化学的计算或高温富燃废气中好。
图2显示了用800℃的入口温度老化的铜/沸石SCR催化剂的样本的类似数据。同样，富燃老化比化学计算的老化或稀燃老化对催化剂更有害。
图2示出了铜/沸石SCR催化剂在脉冲火焰燃烧反应堆上以800℃的温度针对主要为富燃老化循环、主要为化学计算的老化循环或持续稀燃老化循环的老化34小时的NOX转化率与温度的关系。在缓慢的温度上升过程中用500ppm的NO和500ppm的NH3在实验室反应堆上进行评估。
建议的系统存在的问题在于：当发动机的A/F比率是富燃比率时，由于缺少氧气，所以紧密结合的TWC不能转化废气中所有的HC、CO或H2。因此，这些还原剂中的一些将穿过TWC。SCR催化剂中的活性成分是过渡金属。在高温时，这些过渡金属对于氧化H2、CO和HC是活跃的。因此，如果将空气加到富燃废气，则SCR的过渡金属将放热，这会促使过渡金属粗化并降低SCR催化剂的NOX性能。该问题可能的解决方案是在空气注入点和尿素/NH3注入点之间放置另外的氧化催化剂(例如，钯基(Pd-based)TWC)。穿过第一TWC的还原剂将在氧化催化剂(例如，钯基TWC)上被氧化，以防止在SCR的过渡金属上出现放热反应。众所周知，钯催化剂对于热的稀燃废气是耐用的，因此是优选的。在低温时，当尿素被注入到废气中以还原NOX时，尿素或NH3被注入到钯基TWC的下游很重要，以防止钯将NH3氧化成NO或N2。在图3中示出了完整的系统。
图3示出了用于稀燃汽油发动机10的废气20的稀燃NOX后处理系统，该系统包括：点火催化剂30，紧密地结合到发动机10；氧化催化剂150，在点火催化剂30的下游，但在选择性催化还原(SCR)催化剂170的上游。接着，空气注入系统140位于点火催化剂30和氧化催化剂150之间，以保护SCR催化剂170的耐用性。如图3中所阐述的，在该实施例的条件下，还原剂(例如尿素或NH3)被注入SCR 170上游的位置160，以驱动在稀燃条件下选择性地还原NOX的过程。
点火催化剂30通常是用于紧密地结合到发动机10的位置的三元催化剂，优选地含有氧化铝、铑、铂和/或钯，并且还含有用于在化学计算的情况下的三效活性的储氧材料(即，二氧化铈或二氧化铈/氧化锆混合物)。
选择性催化还原催化剂170最好由铜/沸石或铁/沸石配方制成。也可以是具有钨或者钼作为添加剂的氧化钛/氧化钒(vanadia)配方。
位于空气注入系统140之后的氧化催化剂150最好是含有氧化铝和低含量(例如，2至10gpcf(grams per cubic feet))的贵金属(PGM)的三元催化剂，虽然也可使用铂(Pt)以及Pd和Pt的混合物，但优选地使用钯(Pd)。对于氧化催化剂150，由于该催化剂未被用于NOX还原，所以不需要铑。氧化催化剂150可含有储氧材料(例如，二氧化铈或二氧化铈/氧化锆混合物)，以提高耐用性，但这不是必需的。
图4中显示了替代实施例。在该实施例的条件下，为了保护SCR不受热影响，富燃条件在于使用电子控制的换向阀(diverter valve)250，并与被含于旁路臂260中的三元催化剂270结合使用，以在高载运转过程中绕开SCR280。由于SCR 280对于主要在稀燃条件下的NOX还原是有效的，所以在热的富燃条件下，SCR 280不能提供足够的NOX还原。此外，废气温度对于SCR进行有效的NOX控制将会太热。因此，换向阀250可在高载运转过程中引导废气20绕过SCR 280，以保护SCR，从而SCR可在低载和中载运转过程中持续有效地处理NOX排放物，在低载和中载运转过程中，温度的值更利于促使NOX转化。废气20或预测数学模型中的热敏电阻可被用于确定废气20何时应当绕开SCR 280。
根据该系统，当发动机10稀燃运转时，SCR将会在低到中载的过程中转化NOX，当发动机在化学计算的条件或富燃条件下运转时，旁路臂260中的三元催化剂270会提供另外的NOX还原，从而补充在高载情况下点火催化剂30的NOX还原。
旁路臂260中的还原催化剂270最好是含有氧化铝或低含量(例如，2至10gpcf)的铑和钯和/或铂的三元催化剂，还可含有氧化锆。旁路臂260中的还原催化剂270还可含有储氧材料(例如，二氧化铈或二氧化铈/氧化锆混合物)以提高NOX转化率和耐用性。
在另一实施例中，如图5A和图5B所示，在原地制造还原剂。如图5A中所示，在可选的实施例中，使用稀燃NOX吸收装置(LNT)40和SCR 60，从而当发动机10按照稀燃/富燃循环运转时，在富燃清污阶段(rich purgeperiod)由LNT 40产生的NH3被用作下游SCR60的还原剂。与单独的LNT相比，铜基(copper-based)SCR提高了系统的低温性能。在该实施例条件下，空气注入系统50被加在LNT40和SCR60之间，从而当温度高并且A/F比率为富燃时，SCR60被保护。
作为另一实施例，如图5B所示，低含量(low-loaded)的氧化催化剂或TWC 70可被加在空气注入点50和SCR 60之间。同样，由于放热反应将导致SCR 60的热分解(thermal degradation)，所以当发动机富燃运转并且空气被加在SCR之前时，低含量的氧化催化剂或TWC70被加在空气注入点50和SCR 60之间将使SCR 60的放热反应最小化。
在图5A和图5B中示出的实施例的条件下，点火催化剂是被用于紧密地结合到发动机10的位置的三元催化剂，该催化剂最好含有氧化铝、铑和铂和/或钯，并且还含有用于化学计算的条件下的三效活性的储氧材料(即，二氧化铈或二氧化铈/氧化锆混合物)。
在图5A和图5B中示出的实施例的条件下，LNT40最好含有氧化铝、储NOX材料(例如，钡)、铂和铑。钯和储氧材料(例如，二氧化铈或二氧化铈/氧化锆)是可选的。对于该LNT，PGM含量通常是15至100gpcf。
在图5A和图5B的实施例的条件下，SCR催化剂60最好由铜/沸石配方或铁/沸石配方制成。
最后，在图5B的实施例中，低储氧能力(OSC)的TWC催化剂70最好含有氧化铝和低含量(例如，2至10gpcf)的贵金属，最好为钯(Pd)，但是也可使用铂(Pt)或Pd和Pt的混合物。对于低储氧能力(OSC)的TWC催化剂70，由于该催化剂不用于NOX还原，所以不需要铑。虽然非常少量的OSC材料可被用于提高催化剂的耐用性，但是低OSC TWC催化剂70最好不含有储氧材料(例如，二氧化铈或二氧化铈/氧化锆混合物)，以使在富燃清污阶段中由所述催化剂消耗的氨的量最小化。
根据需要，在此公开了本发明的详细的实施例。然而，应当理解，公开的实施例仅是可由不同的可选的形式实施的本发明的示例性实施例。因此，在此公开的具体的功能性细节不应当被解释为限制，而仅作为权利要求的代表性基础和/或用于教导本领域技术人员按照不同方式实施本发明的代表性基础。
虽然已经示出并描述了本发明的实施例，但是这些实施例不旨在示出和描述本发明所有可能的形式。此外，在说明书中使用的词语是描述性的词语而不是限制性的词语，在不脱离本发明的精神和范围的情况下可进行各种改变。

Claims (11)

1、一种还原汽油发动机废气流中的排放物的催化剂系统，该系统包括：
点火催化剂，紧密地结合到发动机；
选择性催化还原催化剂，位于点火催化剂的下游；
还原剂注入系统，位于点火催化剂和选择性催化还原催化剂之间；
空气注入系统，位于点火催化剂和还原剂注入的位置之间，用于将空气注入到处于指定的发动机条件下的废气流内，以提高选择性催化还原催化剂的耐用性。
2、如权利要求1所述的系统，其中，将发动机控制器设置为与空气注入系统结合地运转以将空气注入到在指定的条件下的废气流内，从而提高选择性催化还原催化剂的耐用性。
3、如权利要求1所述的系统，其中，所述空气注入系统是在指定的条件下提供连续的空气流的泵。
4、如权利要求1所述的系统，其中，所述空气注入系统在指定的条件下提供脉冲空气。
5、如权利要求1所述的系统，其中，所述点火催化剂是三元催化剂。
6、如权利要求1所述的系统，其中，在空气注入的位置和还原剂注入的位置之间布置有氧化催化剂，以防止选择性还原催化剂发生放热反应并防止耐用性降低。
7、如权利要求1所述的系统，其中，被注入的所述还原剂是氨。
8、如权利要求1所述的系统，其中，被注入的还原剂是尿素。
9、一种用于提高还原稀燃汽油发动机废气排放物中的排放物的催化剂系统的耐用性的方法，该方法包括下述步骤：
提供催化剂系统，该催化剂系统包括紧密地结合到发动机的点火催化剂以及位于点火催化剂下游的选择性催化还原催化剂；
在会损害选择性催化还原催化剂的耐用性的某些指定条件下将空气注入于点火催化剂和选择性催化还原催化剂之间；
在选择性催化还原催化剂的上游注入还原剂。
10、如权利要求9所述的方法，其中，在空气注入的位置和还原剂注入的位置之间布置有氧化催化剂，以防止选择性还原催化剂发生放热反应并防止耐用性降低。
11、一种还原稀燃汽油发动机废气流中的排放物的催化剂系统，该系统包括：
点火催化剂，紧密地结合到发动机；
选择性催化还原催化剂，位于点火催化剂的下游；
还原剂注入系统，位于点火催化剂和选择性催化还原催化剂之间；
换向阀，位于还原剂注入的位置的下游和选择性催化还原催化剂的上游，所述换向阀连接到包括还原催化剂的旁路臂，该换向阀被用于在高载条件下绕开选择性催化还原催化剂并提高NOx转化率。
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