CN105201600A - 包括NOx储存催化剂和催化烟灰滤清器的排气系统 - Google Patents

包括NOx储存催化剂和催化烟灰滤清器的排气系统 Download PDF

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CN105201600A
CN105201600A CN201510580520.9A CN201510580520A CN105201600A CN 105201600 A CN105201600 A CN 105201600A CN 201510580520 A CN201510580520 A CN 201510580520A CN 105201600 A CN105201600 A CN 105201600A
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A.F.奇费伊
G.M.布朗
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Abstract

本申请涉及包括NOx储存催化剂和催化烟灰滤清器的排气系统。一种用于柴油发动机车辆的排气后处理系统，该系统包括NOx储存催化剂(NSC)和跟随在其下游方向的催化烟灰滤清器(CSF)，其中所述CSF包括氧化催化剂，所述氧化催化剂包括富钯重量比的铂和钯。

Description

包括NOx储存催化剂和催化烟灰滤清器的排气系统
本申请为一项发明专利申请的分案申请，其母案的申请日为2011年3月7日、申请号为201180012610.8(PCT/GB2011/050443)、发明名称为“包括NOx储存催化剂和催化烟灰滤清器的排气系统”。
本发明涉及用于柴油发动机车辆的排气后处理系统，该系统包括NOx储存催化器（NSC）和跟随在其下游方向的催化烟灰滤清器（CSF）。
柴油发动机以某些优点而闻名，这些优点包括低燃料消耗量、高扭矩、以及低一氧化碳（CO）和二氧化碳（CO2）排放。然而，虽然柴油发动机倾向于比汽油发动机产生更少量的管制排放物，但它们也与一些更难处理的排放物联系一起，特别是氮氧化物（NOx，主要是NO和NO2）和颗粒物（PM）。内燃发动机的另一种管制污染物是非燃烧的或未燃烧的（包括部分燃烧的）烃（HC）。
减少发动机排放的方法主要有两种，第一种是发动机设计和管理，第二种是排气后处理。通过研究与开发处理管制排放物的催化方法，排气后处理已经有了很大的发展，并且在与电子发动机管理一起使用时通常能够满足现行排放标准。尽管如此，不断提高的排放规定，结合从环境和全球变暖角度而言要减少燃料消耗和相关的CO2排放的压力，仍不断对发动机和后处理系统的设计提出挑战。
历史上，为车用柴油发动机引入的最早催化后处理是包括沉积在流通式陶瓷或金属蜂窝基材上的铂族金属催化剂（通常为铂）的柴油机氧化催化剂（DOC）。这类DOC能有效地氧化CO和HC，目前被广泛使用。另外，这类DOC可通过同时氧化吸附在碳质颗粒上的（烃的）挥发性有机组分而有效地减少大部分PM。
往往被称作稀燃NOx阱或NOx吸附催化剂（NAC）的串接（in-line）NOx储存催化剂（NSC）的使用目前在稀燃内燃发动机的排气后处理系统中是众所周知的。可能最早的专利公开是Toyota的EP0560991，其记述了怎样通过引入与NOx反应形成硝酸盐的材料（如氧化钡）和NOx转化催化剂（如铂）来构造NOx储存单元。通过调节燃料/空气比（通常称作“拉姆达”或λ）到化学计量比例（λ=1）或浓燃比例（λ<1）来周期性地再生所述NSC。在浓燃偏移（richexcursion）期间，发动机管理提供高浓度的HC，以清除所述NSC中储存的NOx。同时通过与所述催化剂接触将释放的NOx还原成氮气。浓燃清除事件（richpurgeevent）也可称作NSC再生事件。
PM从柴油机排气中的去除通常由某种形式的滤清器或部分滤清器（partialfilter）来实现。在专利文献中已经提出了大量的滤清器设计。目前，现有技术的滤清器是载有PM燃烧催化剂的陶瓷或陶瓷样壁流滤清器，通常称作催化烟灰滤清器（CSF）。人们提出了CSF的许多变体，包括用NOx储存催化剂涂覆滤清器。现有技术的CSF在滤清器前部带有DOC型涂层区而在滤清器后部带有轻负载区（lower-loadedzone）。通常，两个区都是Pt基的。
已经提出了用于柴油机发动机车辆的后处理系统的一种设计，其包括NSC和在其之后的CSF。这种设计在我们的WO2008/075111中有说明，其内容连同其中的参考文献都并入本文。但是，实验证明很难以比较简单和比较便宜的系统满足即将到来的EU6和USTier2Bin5的排放规定。
EP1536111公开了一种在内燃机工作期间，特别是在所述发动机的浓燃操作期间，从排气中除去甲烷（CH4）和一氧化二氮（N2O）的设备和方法，其中所述设备包括用于发动机参数调整的装置、用于NOx还原的包括NOx还原催化剂的装置、和用于还原发动机排气中的甲烷和一氧化二氮的催化剂。在一个优选实施方案中，使用了包括钯和二氧化铈或二氧化锆组分作为颗粒滤清器上的氧存储组分的氮存储还原型催化剂，其中钯用于还原甲烷。
本发明的发明人注意到，用于现代的轻型柴油发动机的排气后处理的一个困难来自低排气温度，特别是在涡轮增压机下游，所述涡轮增压机从排气流中抽取能量从而进一步降低所述气体温度，这将导致催化剂起燃（light-off）困难。他们还注意到，这样的低温度会加重CSF氧化总HC的困难，特别是由于NSC再生所产生的HC有一部分为甲烷，且甲烷构成在再生期间离开NSC的HC的一大部分。
在正常工作条件下甲烷由于其高起燃温度而难以在NSC和CSF上氧化。对于具有位于通道上的Pt催化剂的传统CSF，起燃温度（定义为50%浓度的甲烷反应了的温度）在400℃左右。轻型柴油发动机一般在CSF中不产生这样的温度。轻型柴油机车辆的排气温度只在高速或高负荷行车条件下才到达此区域。因此仍需控制NSC和CSF型系统中的总HC。为避免疑义，NSC用在这里不包括被称作被动NOx吸附器的设备：我们将例如WO2008/047170作为对这样一种被动NOx吸附器的举例说明。
因此，本发明提供一种用于柴油发动机车辆的排气后处理系统，该系统包括NOx储存催化剂（NSC）和跟随在其下游方向的催化烟灰滤清器（CSF），其中所述CSF包括氧化催化剂，所述氧化催化剂包括富钯重量比的铂和钯。所属领域技术人员将可理解，位于传统CSF上的DOC型涂层在发生NSC再生事件的条件下不会氧化大量的甲烷。
此外，本发明还提供一种用于在NSC再生事件期间后处理来自包括排气后处理系统的车用柴油发动机的排气的方法，其中所述排气后处理系统包括NOx储存催化剂（NSC）和跟随在其下游方向的催化烟灰滤清器（CSF），所述方法包括在所述再生事件期间使来自所述NSC的排气从包括富钯重量比的铂和钯的氧化催化剂之上通过。
可取地，将所述氧化催化剂作为部分的、分层的或分区的涂层施加到所述CSF，不过在整个所述CSF上（例如向所有出口通道）施加涂层也包括在本发明的范围之内。就分区的涂层来说，可取的是所述涂层的其余部分为能够在普通的稀燃工作条件下（即不是在浓燃再生事件期间）氧化CO和HC的传统的CSF催化剂。
在优选实施方案中，所述CSF包括含入口通道和出口通道的壁流滤清器。在一个实施方案中，所述入口通道包括铂基氧化催化剂而所述出口通道包括富钯的Pt:Pd氧化催化剂。
或者，可以将所述氧化催化剂布置在一个由所述滤清器的出口端在下游端限定的下游区域，其中所述滤清器的入口端包括一个由所述滤清器的入口端限定的上游区域且其中所述上游区域为铂基氧化催化剂。这种配置可以与壁流滤清器或任何其它滤清器配置结合使用。
布置在入口区域或涂覆在壁流滤清器的入口通道上的传统的铂基CSF催化剂位于布置在出口区域或涂覆在出口通道上的富Pd催化剂上游的配置是有利的，原因在于它能提供更好的热管理并由此提高所述排气后处理系统的效率。特别是，浓燃再生事件产生升高的排气温度。相应地，由于所述滤清器总体上与温度升高的排气接触，所以富Pd催化剂的位置不受温度限制。但是，在一般的稀燃发动机操作（即，再生事件之间）期间排气温度较低，因此铂基催化剂的活性受温度限制。从而，优选将Pt基催化剂设置在一个其在冷启动之后可以尽可能快地实现一氧化碳和烃起燃并可用于处理高速行车时（例如MVEG-B驾驶周期中的EUDC部分）排放的排气的位置。
在所述滤清器以铂基氧化催化剂为特征的实施方案中，优选所述铂基氧化催化剂以富铂的Pt:Pd重量比包括钯。
所述向壁流滤清器及其它滤清器基材上施加涂层以获得部分的、分层的或分区的涂层可以通过所属领域技术人员已知的方法来实现，参见例如我们的WO99/47260或我们在2011年1月4日提交的国际专利申请PCT/GB2011/050005。
所述氧化催化剂可取地包括Pt/Pd组合物。传统的CSF氧化催化剂是基于Pt的，但我们发现Pd是用于氧化甲烷的最好的催化剂。另一方面，纯Pd催化剂非常易受存在于所有柴油机燃料甚至是极低硫的燃料中的硫影响而中毒。目前认为下至约1：10的富Pd的Pt:Pd重量比在本发明中是最有效的。活性催化剂组分的负载量可能需要根据具体的发动机和相关的发动机管理来确定，且还会根据单位面积滤清器基材上的室（cell）的数量和尺寸而变。
沉积的催化剂组合物通常包括传统的载涂层（washcoat）组分。我们认为，甲烷的氧化高度依赖于空气：燃料比，浓燃再生事件期间的条件无助于甲烷的氧化。由此，优选在所述载涂层组合物中并入较高含量的氧储存组分（OSC）组分。最有名的OSC是二氧化铈，其往往以二氧化铈/二氧化锆混合氧化物的形式使用。例如，适合用于本发明的OSC组分负载量为20-50%重量。与之相比，施加到CSF上的传统的催化剂中的OSC组分负载量为0-15wt%。应当理解，所述负载量是指OSC组分的负载量，如果是二氧化铈/二氧化锆50:50，则相应地二氧化铈的量将减半。
可取地，用于本发明的发动机是共轨喷油器型的而非单体喷油器型（PD型）的。我们的初期试验表明，单体喷油器型发动机在NSC再生期间会产生确实极高的甲烷水平（在总HC中有90%的甲烷）。尽管如此，相信本发明仍能提供改善单体喷油器型发动机的HC排放的可能性。
为了更充分地理解本发明，参照附图提供了以下仅作为举例说明的实施例，其中：
图1是显示在暴露于合成排气再生事件8秒和12秒之后离开处于300℃的入口气体温度下的氧化催化剂试样的气体中以ppm表示的总HC减少（slip）的柱状图；和
图2是显示相同氧化催化剂试样在350℃的入口气体温度下的结果的柱状图。
为模拟CSF，使用具有使用传统技术沉积了1.0gin-3的各种催化剂组合物的1英寸x3英寸（2.5cmx7.5cm）的陶瓷流通式基材。在合成催化活性测试(SCAT)设备中将试样暴露于流动的气体，以模拟稀燃条件及随后短暂的（8秒或12秒）浓燃偏移（代表再生）。
将催化剂组合物都以60gft-3沉积到以1gin-3沉积的不同载涂层上。
试样A：在氧化铝载涂层上的2：1的Pt:Pd（非根据本发明）；
试样B：在氧化铝载涂层上的1：2的Pt:Pd；
试样C：在氧化铝载涂层上的1：10的Pt:Pd；
试样D：在50:50的氧化铝：二氧化铈/二氧化锆混合氧化物载涂层上的1：2的Pt:Pd；和
试样E：在50:50的氧化铝：二氧化铈/二氧化锆混合氧化物载涂层上的1：10的Pt:Pd。
稀燃条件气体组成为：8%CO2、12%O2和5%H2O。
浓燃条件气体组成为：8%CO2、0.5%O2、5%H2O、100ppmNO、500ppmCO、1000ppmC1甲烷和以C1碳物质计等量的丙烯。
在8秒或12秒的浓燃偏移（在附图中分别显示为黑色或灰色柱）之前在稀燃条件下在300℃（相当于快速汽车道行车速度下的底置CSF的轻型柴油小客车）和350℃的入口气体温度下使SCAT设备稳定。测量离开所述试样的气体中以ppm计的总HC减少，结果如图1（在300℃下）和图2（在350℃下）所示。
研究所述结果，特别是比较图1中的试样E和试样C，可以看出在试样E中二氧化铈的存在导致在浓燃再生中，特别是在较长的浓燃清除中减少的HC少得多。
图1还表明二氧化铈的存在在较长的浓燃偏移中起重要作用，在8秒和12秒清除的HC减少之间看不出什么差别。
从图2很容易看出，在350℃下，包含比Pt多的Pd、和OSC的试样转化了大部分的HC。

Claims (13)

1.一种用于柴油发动机车辆的排气后处理系统，所述系统包括NOx储存催化剂（NSC）和跟随在其下游方向的催化烟灰滤清器（CSF），其中所述CSF包括氧化催化剂，所述氧化催化剂包括富钯重量比的铂和钯。
2.根据权利要求1所述的系统，其中Pt:Pd重量比为小于1：2。
3.根据权利要求1或2所述的系统，其中Pt:Pd重量比为小于1：10。
4.根据权利要求1、2或3所述的系统，其中所述氧化催化剂包括20-50wt%的量的氧储存组分。
5.根据任一在先权利要求所述的系统，其中所述氧化催化剂包括二氧化铈或二氧化铈-二氧化锆混合氧化物。
6.根据任一在先权利要求所述的系统，其中所述CSF包括含入口通道和出口通道的壁流滤清器。
7.根据任一在先权利要求所述的系统，其中所述氧化催化剂布置在由所述滤清器的出口端在下游端限定的下游区域，其中所述滤清器的入口端包括由所述滤清器的入口端限定的上游区域且其中所述上游区域为铂基氧化催化剂。
8.根据权利要求6所述的系统，其中所述入口通道包括铂基氧化催化剂而所述出口通道包括富钯的Pt:Pd氧化催化剂。
9.根据权利要求7或8所述的系统，其中所述铂基氧化催化剂以富铂的Pt:Pd重量比包括钯。
10.包括柴油发动机和根据任一在前权利要求所述的排气系统的车辆。
11.一种用于在NSC再生事件期间后处理来自包括排气后处理系统的车用柴油发动机的排气的方法，其中所述排气后处理系统包括NOx储存催化剂（NSC）和跟随在其下游方向的催化烟灰滤清器（CSF），所述方法包括在所述再生事件期间使来自所述NSC的所述排气从包括富钯重量比的铂和钯的氧化催化剂之上通过。
12.根据权利要求11所述来减少总羟的方法。
13.根据权利要求11或12所述的方法，其中所述氧化催化剂氧化在所述NSC再生事件期间进入所述CSF的排气中存在的20-90vol%的甲烷。
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