CN103402610A - 在egr回路中具有氨滑移催化剂的排气*** - Google Patents

在egr回路中具有氨滑移催化剂的排气*** Download PDF

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CN103402610A
CN103402610A CN2012800119626A CN201280011962A CN103402610A CN 103402610 A CN103402610 A CN 103402610A CN 2012800119626 A CN2012800119626 A CN 2012800119626A CN 201280011962 A CN201280011962 A CN 201280011962A CN 103402610 A CN103402610 A CN 103402610A
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extraction system
gas extraction
catalyst
egr
gas
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CN103402610B (zh
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G·R·钱德勒
N·R·柯林斯
P·R·菲利普斯
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Johnson Matthey PLC
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Abstract

公开了排放氮氧化物（NOx）和颗粒物质（PM）的车辆稀燃内燃机的排气***。该***包含用于在含氮还原剂存在下还原NOx的NOx还原催化剂、用于将含氮还原剂引入流动的废气的装置、用于从该排气***中流动的废气中除去PM的过滤器，以及用于将过滤器下游的该排气***连接到发动机进气口的低压排气再循环（EGR）回路。该EGR回路包含氨氧化催化剂。

Description

在EGR回路中具有氨滑移催化剂的排气***
发明领域
本发明涉及排放氮的氧化物和颗粒物质的车辆稀燃内燃机的排气***。
发明背景
车辆废气最难以负担的组分之一是氮的氧化物（NOx），其包括一氧化氮（NO）、二氧化氮（NO2）和一氧化二氮（N2O）。NOx的产生对稀燃发动机，如柴油发动机是特别成问题的。为了减轻废气中NOx的环境影响，合意的是消除这些不合意的组分，优选通过不产生其它有害或有毒的物质的方法。
将柴油机废气中的NOx转化为更良性物质的一种方法通常称为选择性催化还原（SCR）。SCR法包括在催化剂的存在下并借助于还原剂将NOx转化为单质氮（N2）和水。在SCR法中，在与催化剂接触前将气态还原剂（通常为无水氨、氨水或脲）添加到废气流中。还原剂被吸收到催化剂上，当气体穿过催化基底或在催化基地上通过时发生NOx还原反应。但是，为使转化效率最大化，通常必须向气流中添加超过化学计量的氨。此类过量的氨如果释放到大气中将对环境有害，由此应当被消除。在传统的排气***中，为此目的在SCR催化剂的下游安装氨氧化催化剂（也称为氨滑移催化剂或“ASC”）。
为了减小排气***所需的空间，通常合意的是设计单个排气组件以执行多于一种的功能。例如，将SCR催化剂施加到过滤器基底上（SCRF）以便通过令一个基底实现两种功能，即通过SCR催化剂催化转化NOx和通过过滤器除去烟炱，由此降低排气处理***的整体尺寸。通常，这两种功能分别单独由SCR和催化烟炱过滤器（CSF）来实施。
废气再循环（EGR）是通过将一部分发动机废气经进气口返回到发动机燃烧室来减少由发动机排放NOx的方法。EGR通过降低燃烧室中的氧气浓度，由此降低燃料燃烧火焰的峰值温度以及通过热吸收来起作用。EGR并非新技术—其自20世纪70年代中期以来已经用于汽油燃料的客车发动机。继汽油应用后，EGR还被引入柴油客车，并自21世纪初开始引入到重型柴油发动机中。
通常，存在两种包含EGR的排气***配置：（i）高压循环EGR，其中废气由涡轮增压器上游再循环以确保废气由前者流入后者；和（ii）低压循环EGR（也称长循环EGR），其中废气通常由颗粒过滤器的下游再循环，使得所有废气在涡轮中使用。过滤器下游的废气压力通常低于进气歧管处的压力，使得废气由前者流向后者的位置。
在使用中，特别是在配置为满足MVEG-A驱动循环的车辆的冷启动过程中，EGR阀设置为将大约50%的废气再循环到发动机。在EGR过程中从发动机排出的废气与从排气***再循环到发动机的废气相比具有较低的氧含量，但不具有较高的NOx含量。
虽然SCRF***与传统的、独立的CSF+SCR催化剂体系相比对于改善的NOx转化而言提供了巨大的优点，通过使用所谓低压EGR获得最大的优点，由此在SCRF后进行该EGR。但是，会遇到一个问题—氨从SCRF中滑移（由于非理想气体或NH3，或NH3源如脲，或由于运行条件的改变—其导致储存的氨从SCRF中释放）。氨或NH3源物类随后进入EGR***。这些物类会对EGR***造成破坏。氨滑移催化剂已经用于防止NH3进入大气（例如经汽车排气管），但还未用于EGR***本身。EGR-ASC应具有高选择性以形成N2并具有低背压。
发明概述
本发明包括排放氮氧化物（NOx）和颗粒物质（PM）的车辆稀燃内燃机的排气***，以及包含该排气***的稀燃内燃机。该***包含用于在含氮还原剂的存在下还原NOx的NOx还原催化剂、用于将含氮还原剂引入到流动的废气中的装置、用于从该排气***中流动的废气中除去PM的过滤器，以及用于将过滤器下游的该排气***连接到发动机进气口的低压排气再循环（EGR）回路。该EGR回路包含氨氧化催化剂。该氨氧化催化剂用于在废气进入发动机前氧化大部分（如果不是全部的话）废气再循环中的氨。由此，该氨氧化催化剂降低了氨滑移的浓度，所述氨滑移来自NOx还原反应、快速升温过程中自催化剂表面的氨释放、或来自于使用化学计量过量的还原剂。
附图概述
图1是本发明的一个实施方案的示意性流程图。
发明详述
本发明是一种排气***，该***包含用于在含氮还原剂的存在下还原NOx的NOx还原催化剂、用于将含氮还原剂引入到流动的废气中的装置、用于从该排气***中流动的废气中除去PM的过滤器，以及用于将过滤器下游的该排气***连接到发动机进气口的低压排气再循环（EGR）回路。该EGR回路包含氨氧化催化剂。
本领域已知的合适的NOx还原催化剂包括选择性催化还原（SCR）催化剂，该催化剂特别可用于选择性催化使用含氮还原剂的NOx还原反应。合适的选择性催化还原催化剂包括过渡金属辅助的分子筛，如铝硅酸盐沸石和硅铝磷酸盐。合适的过渡金属助催化剂包括Cr、Ce、Mn、Fe、Co、Ni和Cu及其任意两种或更多种的混合物。优选的分子筛催化剂包括CuCHA，如Cu-SAPO-34、Cu-SSZ-13和Fe-β沸石，其中Fe存在于分子筛结构的骨架中和/或以其它方式与骨架结构相联（例如与骨架结构离子交换）。Fe-WOx-ZrO2可以用作活性非分子筛SCR催化剂。
用于该***的含氮还原剂可以是氨本身、肼或选自脲（(NH2)2CO）、碳酸铵、氨基甲酸铵、碳酸氢铵和甲酸铵的氨前体。
通过任何适于将还原剂引入废气的装置将该含氮还原剂添加到流动的废气中。合适的装置包括喷射器、喷雾器或进料器，优选是喷射器。此类装置在本领域是公知的。
该***可以包含控制将含氮还原剂引入废气以便在其中还原NOx的装置。在一个实施方案中，该控制装置包含电子控制单元，任选发动机控制单元。此外，该控制装置可以包含位于该NOx还原催化剂下游的NOx传感器。
该***还包含过滤器，优选壁流式过滤器。
该过滤器和NOx还原催化剂可以以任何合适的布局排列。在一个实施方案中，该NOx还原催化剂位于过滤器下游。在此实施方案中，用于将还原剂引入流动的废气的装置合适地位于该过滤器与该NOx还原催化剂之间，
该NOx还原催化剂优选位于该过滤器上，最优选以选择性催化还原过滤器（称为SCRF）的形式。当该过滤器是壁流式过滤器时，该NOx还原催化剂可以配制为渗透该过滤器壁的涂覆涂层（washcoat）。这例如可以通过将该催化剂研磨至≤5μm的平均粒度来实现。在此实施方案中，用于将还原剂引入流动的废气的装置合适地位于该过滤器的上游。
优选地，相对于废气流经该***的方向，可以在该NOx还原催化剂的下游和该EGR的上游布置第二氨氧化催化剂。最优选地，该第二氨氧化催化剂位于该选择性催化还原过滤器的后部，使得该过滤器包含遍布该过滤器的选择性催化还原催化剂，以及相对于废气流经该***的方向，涂有该第二氨氧化催化剂的后部区域。该第二氨氧化催化剂优选包含在金属氧化物如氧化铝上的铂和/或钯。
在一个优选实施方案中，用于将NO氧化为二氧化氮的NO氧化催化剂位于该过滤器和/或该NOx还原催化剂的上游。该NO氧化催化剂优选包含铂族金属，最优选为铂。
该***还包含用于将过滤器下游的该排气***连接到发动机进气口的低压排气再循环（EGR）回路，其中该EGR回路包含氨氧化催化剂（也称为氨滑移催化剂或“ASC”）。
优选应选择该氨氧化催化剂以促进氨的氧化，而非生成NOx或N2O。优选的催化剂材料包括铂、钯或其组合，铂或铂/钯组合是优选的。该氨氧化催化剂优选包含负载在金属氧化物上的铂和/或钯。该催化剂优选安置在大表面积载体上，所述大表面积载体包括但不限于氧化铝。
在某些实施方案中，将该氨氧化催化剂施加到基底上，优选设计为提供大的接触表面与最小背压的基底上。该氨氧化催化剂优选位于流通型整料基底之中或之上，如流通型金属或堇青石蜂巢。例如，优选的流通型整料基底具有每平方英寸大约25至大约300个孔（cpsi）以确保低背压。实现低背压对最小化该氨氧化催化剂对低压EGR性能的影响而言特别重要。
氨氧化催化剂可以以涂覆涂层形式施加到该流通型整料基底上，优选实现大约0.3至2.3g/in3的载量。为了提供进一步的NOx转化，该基底的前部可以仅涂有SCR涂层，后部涂有SCR和氨氧化催化剂组合物，如氧化铝载体上的Pt或Pt/Pd。
根据再一方面，本发明提供包含本发明的排气***的稀燃内燃机。该稀燃内燃机可以是稀燃汽油或柴油发动机，但是该发动机也可以依靠诸如液化石油气、天然气或包括生物燃料或天然气合成油产品的替代燃料来运行。在特定实施方案中，该稀燃内燃机是例如通过柴油提供动力的压燃式发动机。
为了更充分地理解本发明，仅供说明并参照附图提供下列实施例。
实施例
图1是展示布置在排气再循环回路中的氨氧化催化剂组件的包含本发明第一实施方案的排气***的车辆稀燃内燃机的示意图。
参照图1，其显示了包含本发明的排气***10的柴油发动机12。该排气***包含排气管道14，其中后处理组件串列布置。NO氧化催化剂16包含涂有NO氧化催化剂组合物的陶瓷流通型基底整料，所述NO氧化催化剂组合物包含负载在氧化铝基高表面积载体材料上的铂与钯的富铂组合。
包含Cu-SSZ-13选择性催化还原催化剂的涂覆涂层的陶瓷壁流式过滤器20布置在NO氧化催化剂16的下游。任选的氨氧化净化或滑移催化剂36可以涂布在SCR催化剂整料基底的下游端。提供装置（喷射器22）以便将含氮还原剂流体（脲26）从储器24引入到排气管道14携带的废气中。使用阀28控制喷射器22，该阀又受电子控制单元30（通过虚线表示阀控制）的控制。电子控制单元30接收来自位于SCR催化剂下游的NOx传感器32的闭环反馈控制输入。
低压排气再循环回路17包含也受电子控制单元30控制的排气再循环阀18。布置在该排气再循环回路中，ASC19包含涂有负载在氧化铝上的Pt或Pt/Pd组合物的金属流通型基底整料。该ASC19用于氧化以其它方式进入发动机的氨。

Claims (12)

1.排放氮氧化物（NOx）和颗粒物质（PM）的车辆稀燃内燃机的排气***，该***包含用于在含氮还原剂的存在下还原NOx的NOx还原催化剂、用于将含氮还原剂引入流动的废气的装置、用于从该排气***中流动的废气中除去PM的过滤器，以及用于将过滤器下游的该排气***连接到发动机进气口的低压排气再循环（EGR）回路，其中该EGR回路包括氨氧化催化剂。
2.权利要求1的排气***，其中该NOx还原催化剂是包含过渡金属辅助的分子筛的选择性催化还原催化剂。
3.权利要求1的排气***，其中该含氮还原剂是氨、肼或选自脲（(NH2)2CO）、碳酸铵、氨基甲酸铵、碳酸氢铵和甲酸铵的氨前体。
4.权利要求1的排气***，其中该NOx还原催化剂位于该过滤器上。
5.权利要求1的排气***，其中氨氧化催化剂包含负载在金属氧化物上的铂和/或钯。
6.权利要求5的排气***，其中氨氧化催化剂位于流通型整料基底之中或之上。
7.权利要求6的排气***，其中该基底是金属的。
8.权利要求6的排气***，其中该基底每平方英寸横截面积包含大约25至大约300个平行的通道。
9.权利要求6的排气***，其中该基底负载有大约0.3至大约2.3g/in3的氨氧化催化剂。
10.权利要求6的排气***，其中相对于气体流经该基底的方向，该基底具有前部和后部，其中前部负载有选择性催化还原（SCR）催化剂，后部负载有SCR和氨氧化催化剂组合物。
11.权利要求1的排气***，进一步包含相对于废气流经该***的方向布置在该SCRF的下游和该EGR的上游的第二氨氧化催化剂。
12.包含如前述权利要求任一项所述的排气***的稀燃内燃机。
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