CN101321575B - 用于选择性催化还原的多级系统 - Google Patents

用于选择性催化还原的多级系统 Download PDF

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CN101321575B
CN101321575B CN2006800449546A CN200680044954A CN101321575B CN 101321575 B CN101321575 B CN 101321575B CN 2006800449546 A CN2006800449546 A CN 2006800449546A CN 200680044954 A CN200680044954 A CN 200680044954A CN 101321575 B CN101321575 B CN 101321575B
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ammonia
nox
catalytic reduction
selective catalytic
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CN101321575A (zh
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J·J·德里斯科尔
D·M·米拉姆
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Caterpillar Inc
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Abstract

本公开的第一方面包括一种控制氮氧化物排放的方法。该方法可包括产生含有NOx的排气流(11)和将该排气流供给到排气通道(12)。该方法还可包括在第一选择性催化还原催化剂(18)上游的位置处向排气通道供给氨，其中，在所述第一位置处供给的氨的量少于在所述第一位置处还原所有NOx所需的氨的有效量的约90％。此外，可在第一选择性催化还原催化剂下游和第二选择性催化还原催化剂(22)上游的第二位置处向排气通道供给氨。

Description

用于选择性催化还原的多级系统
技术领域
本发明一般涉及排气净化系统，更具体地涉及具有多个(多级)催化剂(催化器)的选择性催化还原系统。
背景技术
选择性催化还原(SCR)提供了一种从用于发动机、工厂和发电厂的化石燃料动力系统中去除氮氧化物(NOx)排放物的方法。在SCR期间，催化剂促进排气氨与NOx之间的反应而生成水和氮气，从而从排气中除去NOx。通常，排气氨在SCR催化剂上游与排气流混合。氨可直接供给到排气流中，或作为可在适当条件下转化成氨的尿素被提供。
为了优化NOx从排气流中的去除，同时阻止可能有害的氨或尿素的释放/逸出，NOx和氨通常以近似1∶1的比例供给。然而，可能难以使氨和流入SCR系统的NOx的量相匹配。此外，即使当比例匹配得很好时，一些NOx可能由于不充分的混合、短的排气通过时间或非最佳的催化剂工作状况而未被还原。因此，需要能更好地除去NOx的改进的SCR系统。
在专利公开WO 2004/058642中公开了一种用于控制NOx排放物的系统，该专利由Valentine在2003年12月17日提交(以下称为’642公开)。’642公开提供了一种多级NOx还原系统。该系统可包括在不同温度范围内有效并具有分别相关的喷射器的多级催化剂。
虽然’642公开的系统可为一些应用提供适当的NOx排放控制，但’642公开的系统可能具有一些缺点。例如，’642公开的系统可能需要还原剂的车载储存，这可能需要很大的空间并且可能有危险。此外，’642公开的系统可能使用比所需更多的还原剂，从而浪费化学制品并可能将还原剂释放到环境中。另外，’642公开的系统可能无法为一些应用提供最优的NOx排放控制。
本发明旨在克服现有技术的NOx排放控制系统的一个或多个缺点。
发明内容
本发明的第一方面包括一种控制氮氧化物排放的方法。本方法可包括产生含有NOx的排气流并将所述排气流供给到排气通道。本方法还可包括在第一选择性催化还原催化剂上游的位置处向所述排气通道供给氨，其中在所述第一位置处供给的氨的量少于在所述第一位置处还原所有NOx所需的氨的有效量的约90％。此外，可在所述第一选择性催化还原催化剂下游和第二选择性催化还原催化剂上游的第二位置处向所述排气通道供给氨。
本发明的第二方面包括一种选择性催化还原系统。该系统可包括排气通道、与所述排气通道流体连通的第一选择性催化还原催化剂和设置在所述第一选择性催化还原催化剂下游并与所述排气通道流体连通的第二选择性催化还原催化剂。该系统还可包括氨产生系统，该氨产生系统构造成在所述第一选择性催化还原催化剂和所述第二选择性催化还原催化剂中至少一者的上游的位置处向所述排气通道供给氨。
本发明的第三方面包括一种NOx排放控制系统。该系统可包括构造成产生含有NOx的排气流的发动机和构造成接收所述含有NOx的排气流的排气通道。第一选择性催化还原催化剂可与所述排气通道流体连通，而第二选择性催化还原催化剂可设置在所述第一选择性催化还原催化剂的下游并与所述排气通道流体连通。氨产生系统可构造成在所述第一选择性催化还原催化剂上游的第一位置处向所述排气通道供给氨。控制单元可构造成监控由所述发动机产生的NOx的量和由所述氨产生系统供给的氨的量以及控制在所述第一位置处供给的氨的量和所述第一位置处的NOx的量。
附图说明
结合在本说明书中并构成本说明一部分的附图示出了本发明的示例性实施例，并与所作说明一同用于解释所公开系统的原理。在附图中：
图1示出发动机和包括根据所公开的示例性实施例的选择性催化还原系统的排气系统。
图2示出发动机和包括根据所公开的示例性实施例的在车上产生氨的选择性催化还原系统的排气系统。
图3示出发动机和包括根据所公开的另一示例性实施例的在车上产生氨的选择性催化还原系统的排气系统。
图4示出发动机和包括根据所公开的另一示例性实施例的在车上产生氨的选择性催化还原系统的排气系统。
具体实施方式
图1示出发动机10和包括根据所公开的示例性实施例的选择性催化还原(SCR)系统16的排气系统14。在发动机10内的燃烧可产生含有NOx的排气流11，该排气流可流入排气系统14的排气通道12。排气流11可朝下游流向SCR系统16的催化剂18、22。
SCR系统16可包括多个SCR催化剂18、22和多个氨供给系统26、30。如图所示，第一SCR催化剂18和第二SCR催化剂22可与排气通道12流体连通，第二SCR催化剂22可设置在第一SCR催化剂18的下游。此外，第一氨供给系统26可构造成在第一SCR催化剂18上游向排气通道12供给氨，而第二氨供给系统30可构造成在第一SCR催化剂18下游和第二SCR催化剂22上游向排气通道12供给氨。
SCR催化剂18、22可包括多个不同的催化剂类型。例如，可选择多种不同的催化剂载体(基底)材料、活化涂层(wash coat)成分和结构。具体的催化剂类型可根据成本、期望的工作温度范围、在使用期间预期产生的NOx的量和/或任意其它适当的因素来选择。此外，第一SCR催化剂18和第二SCR催化剂22可包括不同的催化剂类型。
氨供给系统26、30可包括多种适当的氨供给系统。例如，如图1所示，氨供给系统26、30包括两个流体喷射器。如图所示，这些流体喷射器可构造成向排气通道12供给流体尿素，在排气通道12中尿素可转化成氨。在其它实施例中，至少一个氨供给系统26、30可包括车载氨产生系统，如图2至4所示。
氨供给系统26、30可构造成促进氨和/或尿素与排气流11的混合。例如，氨供给系统26、30可包括绕排气通道12的外周分布的喷射系统。可替换地或附加地，排气通道12可包括其它适当的混合系统。例如，排气通道12可包括一组或多组混合叶片28、32、格栅、穿孔的压力通风系统(plenum)或其它促进氨与排气流11混合的适当结构。
在一些实施例中，第一氨供给系统26可构造成供给一定量的氨，所述量少于在第一SCR催化剂18处除去所有NOx所需的氨的有效量。例如，在一些实施例中，第一氨供给系统26可构造成供给少于氨有效量的约90％、少于氨有效量的约80％、少于氨有效量的约70％或少于氨有效量的60％(的氨)。通过在第一SCR催化剂18处使用少于氨有效量的氨，大部分或所有的氨将与NOx反应，从而防止氨的昂贵的浪费和/或释放。
如果氨仅与NOx反应并且不转化成其它化学物类和/或不会不能用于与NOx反应，则氨的有效量可被认为是用于还原排气中所有NOx所需的氨的量。例如，在一些实施例中，氨的有效量将是用于还原排气中的所有NOx所需的氨的理论配比量(化学计算量，stoichiometric amount)，并且氨供给系统26、30可构造成供给少于还原所有NOx所需的氨的理论配比量的氨。当几乎所有的氨都可用于与NOx反应时(也就是说，没有NOx与其它化学物质反应和/或失去活性或不可用于反应)，可选择该实施例。
应注意，排气流11中的NOx可包括很多NOx种类。典型地，NOx种类可包括一氧化氮(NO)和二氧化氮(NO2)。因此，氨的理论配比量应被认为是将所有NO和NO2转化成氮气和水所需的量。此外，如果使用尿素作为氨源，则所提供的氨的量可被认为是由所提供的尿素的量产生的氨的量。通常，大部分或所有的尿素将被转化成氨。然而，在较冷的工作条件下，可预期会由尿素较慢地生成氨。
在一些实施例中，氨的有效量可大于还原所有NOx所需的氨的理论配比量。例如，在较高的温度(如高于500℃)下，在SCR催化剂18、22内可发生氨的部分氧化，从而将氨转化成其它化学物质并使一些氨无法用于还原NOx。因此，为了计入氨的氧化，在SCR催化剂18、22上游供给的氨的有效量可大于氨的理论配比量。例如，如果大约三分之一的氨产生氧化，则氨的有效量将等于氨的理论配比量的150％。这是正确的，因为在SCR催化剂18、22上游供给的氨仅有三分之二可用于与NOx反应(也就是说，150％的三分之二是理论配比量的100％)。另外，氨的有效量可受到很多其它条件影响，包括例如其它反应物类和/或可暂时或永久地结合氨的排气系统部件的存在。
在一些实施例中，第二氨供给系统30也可构造成供给少于除去残留在第二SCR催化剂22中的所有NOx所需的氨的有效量。例如，在一些实施例中，第二氨供给系统30可构造成供给少于氨的有效量的约90％、少于氨的有效量的约80％、少于氨的有效量的约70％或少于氨的有效量的60％。
应当注意，在第二SCR催化剂22处的NOx的量可比在第一SCR催化剂18处的NOx的量少得多。例如，如果在第一氨供给系统26处提供氨的有效量的80％并且在第一SCR催化剂18处达到90％的转化，则在第一SCR催化剂18处可除去NOx的72％(亦即转化成氮气和水)，而28％会残留。因此，可在第二催化剂22处供给较少量的氨。如果例如又添加氨有效量的80％，则仅需要在第一氨供给系统26处提供的量的大约22％。在一些实施例中，可在第一供给系统26和第二供给系统30处供给少于氨有效量的氨。在其它实施例中，将在第一催化剂18上游供给少于氨的理论配比量的氨，而将在第二催化剂22上游供给大约为氨的理论配比量的氨。
如图所示，SCR系统16包括两个催化剂18、22和两个氨供给系统26、30。然而，可应用任何适当数量的催化剂和氨供给系统。例如，在一些实施例中，可串联设置三个催化剂和三个氨供给系统。第三催化剂可设置在第二催化剂22的下游，而第三氨供给系统可设置在第二催化剂22下游和第三催化剂上游。由于一些NOx已在第一和第二催化剂18、22处通过催化还原除去，所以由第三氨供给系统供给的氨或尿素的量将少于由第一或第二氨供给系统26、30供给的量。此外，在一些实施例中，第三氨供给系统可构造成供给的量少于除去在第三催化剂处残留在排气流中的所有NOx所需的氨或尿素的有效量。在其它实施例中，将在第一催化剂18和/或第二催化剂22上游供给少于氨有效量的氨，而将在第三催化剂的上游供给大约为氨有效量的氨。
此外，排气系统14可包括附加的催化剂、过滤器或其它有利于除去NOx或控制任意排气部件的排放的排气系统部件。例如，如图所示，排气系统14包括上游催化剂34。上游催化剂34可包括例如氧化催化剂，该氧化催化剂可有利于除去某些化学物质和/或有助于产生会在SCR催化剂18、22处促进NOx除去的排气流成分。此外，排气系统14可包括任意其它适当的排气系统部件，例如包括三元催化剂、添加剂供给系统和/或颗粒过滤器。
发动机10和排气系统14还可包括控制单元38，该控制单元可监控和/或控制系统运行。在一些实施例中，控制单元38可监控和/或控制由发动机10产生的NOx的量。控制单元38可包括电控单元，比如车载计算机。然而，可选择任何适当的控制单元。例如，控制单元38可包括机械致动的阀和/或开关的系统，该系统可响应机器的运行而控制由氨供给系统26、30供给的氨量。
此外，控制单元38可根据由发动机10产生的NOx的量来确定应由第一和/或第二氨供给系统26、30供给多少氨。在一些实施例中，控制单元38可根据已知的或测得的发动机运行参数来估算产生了多少NOx。根据估算的NOx产生量供给适当量的氨。此外，在一些实施例中，控制单元38可控制由发动机10产生的NOx的量。例如，可通过改变空气-燃料蒸气比、温度、燃料策略和/或任意其它适当的发动机运行参数来控制由发动机10产生的NOx的量。
在其它实施例中，控制单元38与一个或多个排气监控器42通信。例如，排气监控器42可包括各种传感器，如氧传感器、NOx传感器、温度传感器、氨传感器和/或任意其它适当的传感器或可提供与发动机10和排气系统14内的不同位置处的NOx浓度相关的信息的监控器。控制单元38可根据由传感器42提供的信息来控制氨供给系统26、30的工作，从而使得适当量的氨能供给到排气通道12以除去NOx而不浪费氨。
在一些实施例中，可能希望在发动机10运行期间产生氨。例如，在机动车如卡车运行期间，为SCR运行储存足够量的氨或尿素可能是困难和昂贵的。因此，希望使用车载氨产生系统来产生氨。
图2示出发动机10和排气系统14’，该排气系统包括在车上产生氨的选择性催化还原系统。与在图1的实施例中一样，发动机10可产生含有NOx的排气流11，该排气流流入排气通道并流向多个SCR催化剂18、22。此外，氨产生系统44可构造成在第一SCR催化剂18上游的位置处向排气通道12供给氨，而氨供给系统46可构造成在第一SCR催化剂18下游和第二SCR催化剂22上游的位置处向排气流供给氨。此外，可设置附加的氨供给系统和催化剂。
氨产生系统44可包括任意适当的氨产生系统。例如，氨可由NOx向氨的催化转换产生。因此，如图所示，氨产生系统44可包括NOx源48和一个或多个氨产生催化剂52。NOx源48可提供含有NOx的气流，该气流流过氨产生催化剂52。在氨产生催化剂52处产生的氨与由发动机10产生的含有NOx的排气流11混合，从而NOx的催化去除可在SCR催化剂18、22处发生。NOx源48例如可包括发动机如单缸发动机，该发动机构造成燃烧燃料以产生NOx。NOx源48也可包括任意其它适当的NOx源，比如燃烧器或储存了NOx的供给装置。
氨产生催化剂52可选自多种适当的催化剂类型。例如，氨产生催化剂52可由多种材料制成。在一个实施例中，氨产生催化剂52可包括铂、钯、铑、铱、铜、铬、钒、钛、铁或铯中的至少一种。也可使用这些材料的组合，并且可根据成本、所用燃料的种类、期望的空气-燃料蒸气比或为了与环境标准相符来选择催化剂材料。也可选择催化剂的具体类型以控制NOx向氨的转化效率。此外，可根据由NOx源48产生的NOx的量和/或在选定运行条件下的催化剂温度来选择催化剂。
催化剂的工作可受到多种不同因素的影响。例如，其它化学物质在周围排气中的存在、催化剂温度和/或被排气化学物质的污染可影响催化剂的工作。在本发明的一些实施例中，可通过使用冷却系统56如涡轮增压器、气体-空气冷却器或气体-水冷却器冷却由NOx源48产生的含有NOx的气流50来控制氨产生催化剂52的温度。此外，可通过控制NOx源48的运行、通过使用添加剂供给装置或通过使用位于氨产生催化剂52上游的一个或多个附加催化剂60来控制其它化学物类在排气流18中的存在。
如所述，排气系统14’可包括位于第一SCR催化剂18下游和第二SCR催化剂22上游的氨供给系统46。如图2所示，第二SCR催化剂22包括用于向排气系统供给液体尿素或氨的喷射器。或者，第二氨供给系统46可包括车载氨产生系统。例如，图3示出发动机10和具有车载氨产生系统44’的排气系统的第二实施例。如图所示，车载氨产生系统44’包括NOx源48’和氨产生催化剂52’。此外，系统包括两个排气通道100、104，所述排气通道构造成向第一SCR催化剂18和第二SCR催化剂22的上游位置供给氨。系统还包括用于控制氨流过排气通道100、104的阀系统96。或者，排气系统可包括多个车载氨产生系统，这些车载氨产生系统构造成向所选定的排气系统位置供给期望量的氨。
在一些实施例中，可使用单个发动机作为用于产生氨的NOx源和主作业机械动力源。例如，图4示出另一发动机10’和排气系统14”，该排气系统包括根据所公开的示例性实施例的在车上产生氨的选择性催化还原系统。单个发动机10’可用作用于在车上产生氨的NOx源和机械动力源。发动机10’可包括第一气缸组64和第二气缸组68。第一气缸组64可产生含有NOx的第一排气流72，该第一排气流可用于通过氨产生系统44”产生氨。第二气缸组68将产生含有NOx的第二排气流76。第一气缸组64和第二气缸组68均可对作业机械如卡车的总发动机功率有所贡献。
如所述，第一气缸组64和第二气缸组68可位于单个发动机10’上。如所示，第一气缸组64包括单个气缸，而第二气缸组68包括三个气缸。然而，第一和第二气缸组64、68可包括任意适当数量的气缸。
第一气缸组64和第二气缸组68可具有不同的运行特性。例如，与第二气缸组68相比，第一气缸组64可具有不同的空燃比，可采用不同的燃烧策略，可包括排气添加剂供给装置，可具有不同的压缩比，可具有不同的气缸尺寸，可包括不同数量的气缸，和/或可在不同的温度下运行。在一些实施例中，第一气缸组64可构造成对于给定量的所用燃料使NOx产量最大，从而通过氨产生系统44”增加氨产量。
来自第二气缸组68的含有NOx的排气流76可流入排气通道88。此外，如所示，车载氨产生系统44”构造成向第一SCR催化剂18上游的排气通道88供给氨。此外，氨供给系统92可构造成在第一SCR催化剂18下游和第二SCR催化剂22上游的位置向排气通道88供给氨。在其它实施例中，氨产生系统44”可构造成使用具有用于控制排气流的系统的分支排气通道在多个位置向排气通道88供给氨。或者，可在第一SCR催化剂18上游和/或第二SCR催化剂22上游及第一SCR催化剂18下游的位置处使用多个氨产生系统。
应注意，如图2至4所示，包括车载氨产生系统的SCR系统也可由控制单元38控制。如参照图1所述，控制单元38可与多个排气监控器42通信，所述排气监控器构造成提供与排气状况相关的信息，例如温度、氧浓度、NOx浓度和/或氨产量。
另外，如上所述，车载氨产生系统44、44’、44”可用作用于SCR催化剂18、22的氨供给系统。在本发明的一些实施例中，车载氨产生系统可构造成供给少于在排气系统内的选定位置除去NOx所需的氨有效量的氨。例如，如参照图1所述，氨产生系统44、44’、44”可构造成供给少于氨有效量的约90％、少于氨有效量的约80％、少于氨有效量的约70％或少于氨有效量的约60％的氨。
工业适用性
本发明提供了一种具有用于SCR系统的多级喷射器的排气排放控制系统。该系统可用在需要SCR的所有排气系统中。
SCR系统可提供一种用于在保持高的燃料效率的同时控制NOx排放的有效方法。然而，SCR系统需要氨，氨可由在车上产生氨或者由氨或尿素的储存来提供。在车上产生氨会消耗大量燃料和/或其它化学物质，这会降低发动机的总体燃料效率和成本效率。此外，为了后来的喷射而储存氨或尿素可能是昂贵或危险的。另外，目前尚没有适当的基础设施来供给尿素或氨以供公路车辆储存和消耗。
本发明的系统可提供比单催化剂SCR系统更高的NOx转化效率。通常，燃料效率越高的发动机运行将产生越高水平的NOx。因此，由多级SCR系统带来的更高的NOx转化效率将使得发动机更有效率地运行，同时保持适当的NOx排放水平。这将很好地控制NOx排放，同时降低用于发动机运行的燃料成本。
另外，本发明的系统可利用SCR系统来改善NOx排放控制，同时还降低用于SCR运行所需的氨或尿素的量。该系统包括具有两个或多个串连的氨供给系统和SCR催化剂的多级氨供给和催化系统。由于通过SCR还原NOx会被氨与含有NOx的排气流混合的能力和/或催化剂效率所限制，所以本发明的至少一个氨供给系统可构造成供给少于除去NOx所需的氨有效量的氨。此后，一个或多个下游的氨供给系统和SCR催化剂将除去另外的NOx。多级系统可在使用过量氨或尿素的风险极小的情况下除去大量的NOx。这将很好地控制NOx排放，同时使SCR运行成本最低。
本领域技术人员显然清楚，可对所公开的系统和方法作出各种修改和变型而不会脱离本发明的范围。鉴于本说明书和对本文所公开的实施例的实践，所公开的系统和方法的其它实施例对于本领域技术人员而言也是显而易见的。本说明书和示例应被认为仅仅是示例性的，本发明的真正范围由所附权利要求及其等同物指明。

Claims (4)

1.一种控制氮氧化物排放的方法，包括：
产生含有NOx的排气流(11)；
将所述排气流供给到排气通道(12)；
通过至少一个发动机气缸内的燃料的燃烧来产生含有NOx的第二排气流，并将所述第二排气流中的至少一部分NOx转化成氨，以产生含氨排气流；
在第一选择性催化还原催化剂(18)上游的第一位置处向所述排气通道供给所述含氨排气流，其中，在所述第一位置处供给的氨的量少于在所述第一位置处还原所有NOx所需的氨的有效量的90％；并且
在所述第一选择性催化还原催化剂下游和第二选择性催化还原催化剂(22)上游的第二位置处向所述排气通道供给尿素。
2.根据权利要求1所述的方法，其特征在于，在所述第一位置处供给的氨的量少于在所述第一位置处还原所有NOx所需的氨的有效量的80％。
3.一种选择性催化还原系统(16)，包括：
排气通道(12)；
与所述排气通道流体连通的第一选择性催化还原催化剂(18)；
设置在所述第一选择性催化还原催化剂下游并与所述排气通道流体连通的第二选择性催化还原催化剂(22)；
包括构造成产生含NOx排气流的至少一个发动机气缸和构造成将所述含NOx排气流中的至少一部分NOx转化成氨的至少一个催化剂的氨产生系统(44)，所述氨产生系统构造成在所述第一选择性催化还原催化剂上游的第一位置处向所述排气通道供给氨，使得在所述第一位置处供给的氨的量少于在所述排气通道内还原所有NOx所需的氨的有效量的90％；以及
构造成在所述第一选择性催化还原催化剂下游和所述第二选择性催化还原催化剂上游的第二位置处供给尿素的尿素供给系统。
4.一种NOx排放控制系统，包括：
如权利要求3所述的选择性催化还原系统；
构造成产生含有NOx的排气流的发动机；以及
控制单元(38)，该控制单元构造成监控由所述发动机产生的NOx的量和由所述氨产生系统供给的氨的量以及控制在所述第一位置处供给的氨的量和所述第一位置处的NOx的量，使得氨的量少于在所述第一位置处还原所有NOx所需的氨的有效量的90％。
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