CN103402609A - 包括NOx还原催化剂和EGR回路的排气系统 - Google Patents

包括NOx还原催化剂和EGR回路的排气系统 Download PDF

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CN103402609A
CN103402609A CN2012800097063A CN201280009706A CN103402609A CN 103402609 A CN103402609 A CN 103402609A CN 2012800097063 A CN2012800097063 A CN 2012800097063A CN 201280009706 A CN201280009706 A CN 201280009706A CN 103402609 A CN103402609 A CN 103402609A
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extraction system
gas extraction
reducing agent
adsorbent
catalyst
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G·R·钱德勒
A·N·M·格林
S·D·雷德
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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系统。该系统包含用于在还原剂存在下还原NOx的NOx还原催化剂、用于将还原剂引入流动的废气的装置和选自烃还原剂、含氮还原剂、氢及其任意两种或多种的混合物的还原剂的来源、用于从该排气系统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系统连接到发动机进气口的低压排气再循环（EGR）回路。该EGR回路包括包含NO吸附剂的NOx吸附催化剂（NAC）。

Description

包括NOx还原催化剂和EGR回路的排气系统
发明领域
本发明涉及排放氮的氧化物和颗粒物质（PM）的车辆稀燃内燃机的排气系统。
发明背景
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氮氧化物（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的排气系统配置：（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系统再循环到发动机的废气相比具有较低的氧含量，但具有较高的NOx含量。
WO2008/047170公开了减少包含氧化一氮（NO）的贫气流中存在的氮氧化物（NOx）的方法，该方法包括以下步骤：（i）在低于200℃的温度下在包含钯和氧化铈的吸附剂中从贫气流中净吸附NO本身；（ii）在200℃及更高的温度下在贫气流中由该NO吸附剂热净解吸NO；和（iii）在除NO吸附剂之外的催化剂上用选自烃还原剂、含氮还原剂、氢及其任意两种或更多种的混合物的还原剂催化还原NOx。还公开了一种还原包含NO的贫气流中的NOx的系统，该系统包括在低于200℃的温度下从贫气流中吸附NO本身的吸附剂、用于在200℃及更高的温度下使NO吸附剂与贫气流接触由此从该NO吸附剂中解吸NO的装置，以及包含NO还原催化剂和选自烃还原剂、含氮还原剂、氢及其任意两种或更多种的混合物的还原剂的来源的用于还原从该NO吸附剂中解吸的NO的装置，其中该NO吸附剂包含钯和氧化铈。
我们现在提出一种可以在法定驱动循环（如欧洲MVEG-A驱动循环）中和在真实世界条件下改善NOx转化的排气系统配置，其相对于现有的商业排气系统配置可以降低来自车辆稀燃内燃机的NOx排放。
发明概述
本发明包括排放氮氧化物和颗粒物质（PM）的车辆稀燃内燃机的排气系统，以及包含该排气系统的稀燃内燃机。该系统包含NO还原催化剂和选自烃还原剂、含氮还原剂、氢及其任意两种或更多种的混合物的还原剂的来源、用于从该排气系统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系统连接到发动机进气口的低压排气再循环（EGR）回路。该EGR回路包括包含NO吸附剂的NOx吸附催化剂（NAC）。这种配置的优点在于NOx还原催化剂在低于大约200℃的温度下通常对NOx还原是惰性的。此外，当该NOx还原催化剂使用脲还原剂还原NOx时，直到将废气充分升温至足以将脲分解为CO2和氨可能才可以注入脲，否则存在脲的固体沉积物堵塞下游NOx还原催化剂和/或脲喷射器的风险。通过在NOx还原催化剂对NOx还原为活性时用热的方法，即被动地释放储存的NO回到废气中之前，在低于该NOx还原催化剂的所需点火温度的温度下在排气再循环回路中吸附NO，该系统总体上排放更少的NOx，增加了本领域技术人员满足相关排放标准的设计方案。
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
本发明是一种排气系统，该系统包含NO还原催化剂和选自烃还原剂、含氮还原剂、氢及其任意两种或更多种的混合物的还原剂的来源、用于从该排气系统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系统连接到发动机进气口的低压排气再循环（EGR）回路。该EGR回路包括包含NO吸附剂的NOx吸附催化剂（NAC）。
该过滤器优选是壁流式过滤器。
在一个实施方案中，该NO吸附剂由钯与氧化铈或含有铈和至少一种其它过渡金属的混合氧化物或复合氧化物组成，而在另一实施方案中，该NO吸附剂包括分散在二氧化铈或含有铈和至少一种其它过渡金属的混合氧化物或复合氧化物上的钯。在一个特定实施方案中，混合氧化物或复合氧化物中的至少一种其它过渡金属是锆。
该NO吸附剂中合适的钯载量可以为0.1至200g/ft-3（0.0035至7.1g/L）。在一个实施方案中，氧化铈或含有铈的复合氧化物上的钯载量为0.1至200g/ft-3（0.0035至7.1g/L），如0.5至150g/ft-3（0.018至5.3g/L）或1至120g/ft-3（0.035至4.2g/L）。
本文中定义的“复合氧化物”是指包含至少两种元素的氧化物的主要为无定形的氧化物材料，其并非由至少两种元素组成的真正的混合氧化物。
包含钯和氧化铈的材料可以通过已知方法获得，所述方法包括但不限于浸渍、初始含浸技术和共沉淀。可以根据EP0602865中公开的方法获得共沉淀材料。
在可用于但不限于处理稀燃内燃机、尤其是车辆发动机排放的NOx的另一实施方案中，该NO吸附剂与用于在高于大约200℃的温度下净吸附NOx并在高于250℃的温度下热净解吸NOx（即在高于大约200℃至最高大约250℃下净吸附）的可热再生NOx吸附剂结合，该可热再生NOx吸附剂包含铂和金属氧化物。在实施方案中，可热再生NOx吸收剂可以包含分散在氧化铝和/或氧化锆上的铂。这种实施方案的优点在于能够将净NOx解吸推迟到更高的温度（高于大约250℃的温度，如255℃、260℃、265℃或270℃），在该温度下相关NO还原催化剂（例如使用含氮还原剂的选择性催化还原催化剂）对NO还原而言比在刚好高于200℃的温度下更具有活性，或者其使得能够使用氨前体如脲——其在更高的温度下可以更容易地水解或热解。
本文中所用术语“吸收”和“吸附”及其任何衍生形式可以互换使用，并应相应地解释本说明书。
该NO吸附剂和可热再生NOx吸收剂可以以提供此益处的任何合适配置布置。例如，在一个实施方案中，流通型基底整料在基底整料的入口端用该NO吸附剂涂布一个区域，并在基底整料的出口段用可热再生NOx吸收剂涂布一个区域。或者，该NO吸附剂存在于基底整料上的下层中，可热再生NOx吸收剂存在于覆盖该下层的层中。
本领域已知的合适的NOx还原催化剂包括稀燃NOx催化剂（也称作烃-SCR催化剂），其可以使用烃和/或氢作为还原剂，或包含碱土金属或碱金属NOx吸附剂组分和适宜地包含铂的NO氧化催化剂组分，以及任选NOx还原催化剂组分，如铑的NOx捕集催化剂。在一个优选实施方案中，NOx还原催化剂是选择性催化还原（SCR）催化剂，还原剂是含氮还原剂。
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，但是如果进行排列以避免还原剂在过滤器上燃烧的话，其还可以位于该NOx还原催化剂的上游。
在另一实施方案中，该NOx还原催化剂位于过滤器上。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。
在一个优选实施方案中，用于将NO氧化为二氧化氮的氧化催化剂位于该过滤器和/或该NOx还原催化剂的上游。
优选地，该NOx还原催化剂选择性催化使用含氮还原剂的NOx的还原。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以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。
用于该系统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。
用于本发明的系统或方法的还原剂是合适的烃还原剂、含氮还原剂或氢。在本发明的系统的优选用途中使用烃还原剂的配置中，该烃还原剂可以是为发动机提供动力的烃燃料。当该还原剂是烃燃料时，其可以合意地裂化该燃料以形成更短链的烃类以促进更有效的NOx还原。在这方面，Pd/CeO2是用于裂化烃燃料的特别有效的催化剂。
含氮还原剂可以包括氨本身、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。例如可以通过令烃燃料与合适的重整催化剂接触，或者当该气体包含二氧化碳和水时通过令该气流与合适的水汽变换催化剂接触而原位生成氢气。
通过任何适于将还原剂引入废气的装置将该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。
该系统可以包含控制将还原剂引入废气以还原其中的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NO还原催化剂下游的NOx传感器。
根据另一方面，本发明提供包含本发明的排气系统的稀燃内燃机。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。在一个具体实施方案中，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可热再生NO吸附剂的包含本发明第一实施方案的排气系统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系统10的柴油发动机12。该排气系统包含排气管道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比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（washcoat）的陶瓷壁流式过滤器20布置在NO氧化催化剂16的下游。氨氧化净化或滑动（slip）催化剂36涂布在SCR催化剂整料基底的下游一端。或者，该氨滑动催化剂可以涂布在位于SCR催化剂下游的单独基底上（未显示）。提供装置（喷射器22）以便将还原剂流体（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，NO吸附剂19包含涂有NO吸附剂组合物的陶瓷流通型基底整块，所述NO吸附剂组合物包含负载在二氧化铈上的钯，该吸附剂组合物在最高大约200℃的温度下从稀燃废气中净吸附NO，并在高于大约200℃的温度下在稀燃废气中净解吸NO。
在使用中，负载在二氧化铈NO吸附剂19上的钯在最高大约200℃的温度下从排气再循环回路中流动的废气中净吸附NO，例如在MVEG-A欧洲驱动循环中的冷启动之后，或在产生更冷的废气的驱动条件（例如在交通中的长时间空转）期间。当排气再循环系统中的废气温度升高时，NO被热（即被动地）解吸并通到发动机进气口，并且在从发动机中排出后，一定比例的衍生自解吸的NO的NOx在衍生自经喷射器22注入的脲的氨的存在下在SCR催化剂20上被还原。氨滑动催化剂36氧化NH3（否则将排放至大气中）。

Claims (20)

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系统，该系统包含用于在还原剂存在下还原NOx的NOx还原催化剂、用于将还原剂引入流动的废气的装置和选自烃还原剂、含氮还原剂、氢及其任意两种或更多种的混合物的还原剂的来源、用于从该排气系统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系统连接到发动机进气口的低压排气再循环（EGR）回路，其中该EGR回路包括包含氧化一氮（NO）吸附剂的NOx吸附催化剂（NAC）。
2.如权利要求1所述的排气系统，其中该NO吸附剂由钯与氧化铈或含有铈和至少一种其它过渡金属的混合氧化物或复合氧化物组成。
3.如权利要求1或2所述的排气系统，其中该NO吸附剂包括分散在二氧化铈或含有铈和至少一种其它过渡金属的混合氧化物或复合氧化物上的钯。
4.如权利要求2或3所述的排气系统，其中混合氧化物或复合氧化物中的至少一种其它过渡金属是锆。
5.如权利要求1、2、3或4所述的排气系统，其中该NO吸附剂具有0.1至200g/ft-3的钯载量。
6.如前述权利要求任一项所述的排气系统，其中该NO吸附剂与用于在高于200℃的温度下净吸附NOx并在高于250℃的温度下净解吸NOx的可热再生NOx吸附剂结合，该可热再生NOx吸附剂包含铂和金属氧化物。
7.如权利要求6所述的排气系统，其中该可热再生NOx吸收剂包含分散在氧化铝和/或氧化锆上的铂。
8.如权利要求6或7所述的排气系统，其中该NO吸附剂存在于下层中，可热再生NOx吸收剂存在于覆盖该下层的层中。
9.如前述权利要求任一项所述的排气系统，其中该NOx还原催化剂位于过滤器下游。
10.如权利要求9所述的排气系统，其中用于将还原剂引入流动的废气的装置位于该过滤器与该NOx还原催化剂之间。
11.如权利要求1至9任一项所述的排气系统，其中该NOx还原催化剂位于过滤器上。
12.如权利要求11所述的排气系统，其中用于将还原剂引入流动的废气的装置位于该过滤器的上游。
13.如前述权利要求任一项所述的排气系统，包含位于该过滤器和/或该NOx还原催化剂上游的用于将NO氧化为二氧化氮的氧化催化剂。
14.如前述权利要求任一项所述的排气系统，其中该NOx还原催化剂选择性催化使用含氮还原剂的NOx的还原。
15.如前述权利要求任一项所述的排气系统，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。
16.如前述权利要求任一项所述的排气系统，包含控制将还原剂引入废气以还原其中的NOx的装置。
17.如权利要求16所述的排气系统，其中该控制装置包含电子控制单元。
18.如权利要求16或17所述的排气系统，其中该控制装置包含位于该NO还原催化剂下游的NOx传感器。
19.包含如前述权利要求任一项所述的排气系统的稀燃内燃机。
20.如权利要求19所述的压燃式发动机。
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