CN110462176B - 从发动机废气中除去有害化合物的方法和系统 - Google Patents

从发动机废气中除去有害化合物的方法和系统 Download PDF

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CN110462176B
CN110462176B CN201880019621.0A CN201880019621A CN110462176B CN 110462176 B CN110462176 B CN 110462176B CN 201880019621 A CN201880019621 A CN 201880019621A CN 110462176 B CN110462176 B CN 110462176B
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exhaust gas
catalyst
nitrogen dioxide
engine exhaust
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P·L·T·加布里埃尔森
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Umicore Corp And Lianghe Co
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Abstract

本发明涉及用于在冷启动条件下从发动机废气中除去氮氧化物、挥发性有机化合物和颗粒物的方法和系统。

Description

从发动机废气中除去有害化合物的方法和系统
本发明涉及用于减少在发动机废气中存在的氮氧化物(NOx)和颗粒物的排放的方法和系统。具体地，本发明的方法和系统在发动机的冷启动期间提供NOx的改善的减少。
通常，具有贫燃发动机的车辆或固定式发动机的废气清洁系统配备有氧化催化剂、颗粒过滤器和催化剂，在还原剂的存在下用于选择性还原NOx(SCR)。
在挥发性有机化合物、一氧化氮和一氧化碳以及SCR催化剂的氧化中具有活性的氧化催化剂是本领域中已知的，并且公开于许多出版物中。
已知SCR催化剂的问题是在低于250℃的废气温度下的相对低效率。
具体地，冷启动排放减少是认证发动机时的一个重要问题。已探索到不同的方法，它们中的大多数基于通过不同的发动机措施加热废气，但常常导致恶化的燃料效率。
已知SCR反应能够显著加速，并且能够通过所谓的“快速”SCR反应在废气中的等量NO和NO2下显著提高低温活性：
2NH3+NO+NO2→2N2+3H2O。
增加NO2的量的通常方法是使用SCR催化剂上游的氧化催化剂来将NO氧化为NO2。然而，问题在于氧化催化剂在冷启动条件下的效率较差，并且在低于200℃的废气温度下形成非常低含量的NO2。
本发明基于在废气通道中的废气清洁系统外部形成NO2，并且以促进快速SCR反应的量将制备的NO2注入发动机废气中。NO2能够通过在第一步骤中由含有贵金属的催化剂将NH3氧化为NO而由NH3形成，并且随后在后续步骤中将NO2氧化。
因此，本发明在第一方面提供了从发动机废气中除去氮氧化物、挥发性有机化合物和颗粒物的方法，所述方法包括以下步骤：
在以原样或其前体形式加入到所述发动机废气中的氨的存在下，使所述发动机废气按顺序通过氧化催化剂、通过颗粒过滤器和用于选择性还原氮氧化物的催化剂；
在低于250℃的发动机废气温度下，将含有二氧化氮的排放气体注入用于选择性还原氮氧化物的催化剂上游的发动机废气中；
通过以下步骤提供含有二氧化氮的排放气体：
在氧化催化剂的存在下，用含氧气氛将氨催化氧化为包含一氧化氮和氧气的排放气体；
将所述排放气体冷却至环境温度，并且将所述冷却的排放气体中的一氧化氮氧化为二氧化氮。
用于从压缩点火发动机中清洁发动机废气的清洁方法和系统本身是本领域中已知的，包括使发动机废气按顺序通过氧化催化剂(DOC)、通过颗粒过滤器(PDF)和催化剂，以在加入发动机废气中的氨的存在下像这样或以尿素前体的形式选择性催化还原氮氧化物(SCR)。
如前文所述，已知方法和系统的问题使在低于250℃的废气温度的冷启动条件下，SCR催化剂的相对低效率。该问题通过本发明解决，其中在冷启动温度期间将NO2注入发动机废气中以促进“快速”SCR反应。该反应负责通过NO2促进低温SCR。
当离开发动机时，含于发动机废气中的NO在250℃以上通过与DOC接触而被氧化为NO2。因此，在250℃的温度以上，所有形成的NO2的量均能够用于过滤器的被动烟尘再生和快速SCR反应。
因此，当气体温度达到250℃时，将NO2注入发动机废气中可能被破坏。
通常在含氧气氛如空气的存在下，在介于250℃和800℃之间的反应温度下，在具有贵金属催化剂(通常为铂或铂与其它贵金属的合金)作为微量组分的反应器中进行氨至NO的氧化。
为了提供所需的反应温度，氧化反应器能够通过例如电加热或感应加热来加热。
在一个实施方案中，含氧气氛包括热再循环发动机废气，其提供氧化反应器加热负荷的附加部分。
通过在第一步骤中由NH3与含有贵金属的催化剂接触而氧化由NH3形成的NO随后通过将气体冷却至环境温度以在上述反应方案中朝向形成NO2推动平衡反应
Figure GDA0003146981160000031
NO2来在来自第一步骤的含有NO的排放气体中氧化为NO2。
如本文所用，术语“环境温度”应意指在采用本发明的方法和系统的车辆或固定式发动机周围存在的任何温度。通常，环境温度将介于—20℃和40℃之间。
含有NO的排放气体的冷却和氧化能够在老化反应器中进行，所述老化反应器的尺寸被设定成使得气体的停留时间为约1分钟或更长。
在一个实施方案中，氧化反应在催化剂的存在下进行，所述催化剂促进NO至NO2的氧化。那些催化剂是本领域中已知的，并且包括TiO2上的Pt、SiO2上的Pt和活性炭。
如前文所述，所期望的快速SCR反应需要等量的NO和NO2。因此，在低于250℃的温度的冷启动条件下注入发动机废气中的NO2的量被控制为在通向SCR催化剂单元的入口处导致发动机废气中45体积％至55体积％的氮氧化物含量为NO2。
NO2能够被用于氧化捕集在DPF上的烟尘颗粒，并且可用于DPF的被动再生。
因此，在本发明的一个实施方案中，将含有二氧化氮的排放气体注入颗粒过滤器的上游。
为了通过燃烧积聚的烟尘促进可靠的DPF再生并同时除去烃和一氧化碳，DPF优选设置有催化涂层。
在烟尘燃烧时有活性的催化剂本身是本领域中已知的。此类催化剂的示例为与用ZrO2稳定的CeO2或氧化铝上的铂组合的钯。
在250℃以上，废气中的NO通过与DOC接触而被氧化为NO2。所形成的NO2被用于DPF的被动再生。因此，在250℃的温度以上，所有形成的NO2的量均能够被用于过滤器的被动烟尘再生并促进快速SCR，并且含有NO2的气体的注入被破坏。
在另一方面，本发明提供了一种在根据本发明的方法中使用的系统。
所述系统在发动机废气通道内按顺序包括：
氧化催化剂单元，所述氧化催化剂单元用于将挥发性有机化合物和一氧化碳氧化为二氧化碳，并且将水和氮氧化物氧化为二氧化氮；
颗粒过滤器；
催化剂，所述催化剂用于选择性还原氮氧化物；
在用于选择性还原氮氧化物的所述催化剂上游的注入装置，所述注入装置用于将氨或尿素溶液注入所述发动机废气通道中；
在用于选择性还原氮氧化物的所述催化剂上游的注入装置，所述注入装置用于注入含有二氧化氮的排放气体；以及在所述废气通道之外的氨氧化催化剂；以及
装置，所述装置用于从所述氨氧化催化剂冷却和氧化含有一氧化氮的排放气体，所述装置在其出口端处连接到用于注入含有二氧化氮的排放气体的所述注入装置。
在本发明的一个实施方案中，用于注入含有二氧化氮的排放气体的注入装置被布置在颗粒过滤器的上游。用该实施方案，在发动机废气达到上游氧化催化剂产生足量NO2的温度之前，可能在更低的温度下被动再生颗粒过滤器。
如上所述，NO至NO2的氧化反应需要含有NO的气体的停留时间为约1分钟。通常为1-2分钟。
这能够优选在将冷却装置和氧化装置成形为螺旋卷绕管时实现，所述螺旋卷绕管具有导致气体穿过管所需的停留时间的长度。
在另一个实施方案中，用于冷却和氧化含有一氧化氮的排放气体的装置设置有氧化催化剂设置有氧化催化剂，所述氧化催化剂促进NO至NO2氧化的氧化。
在另一个实施方案中，颗粒过滤器用在烧掉烟尘时有活性的催化剂催化。

Claims (12)

1.一种用于从发动机废气中除去氮氧化物、挥发性有机化合物和颗粒物的方法，所述方法包括以下步骤：
在以原样或以其前体形式加入到所述发动机废气中的氨的存在下，使所述发动机废气按顺序通过氧化催化剂、通过颗粒过滤器和用于选择性还原氮氧化物的催化剂；
在低于250℃的发动机废气温度下，将含有二氧化氮的排放气体注入所述用于选择性还原氮氧化物的催化剂上游的发动机废气中；
通过以下步骤提供所述含有二氧化氮的排放气体：
在氧化催化剂的存在下，用含氧气氛将氨或其前体催化氧化为包含一氧化氮和氧气的排放气体；
将所述排放气体冷却至环境温度，并且将所述冷却的排放气体中的一氧化氮氧化为二氧化氮，
其中所述含有二氧化氮的排放气体在废气通道中的废气清洁系统的外部形成。
2.根据权利要求1所述的方法，其中所述含氧气氛包含发动机废气。
3.根据权利要求1所述的方法，其中所述氧气氛为环境空气。
4.根据权利要求1所述的方法，其中将含有二氧化氮的排放气体注入所述颗粒过滤器的上游。
5.根据权利要求1所述的方法，其中将所述含有二氧化氮的排放气体在通向所述用于选择性还原氮氧化物的催化剂的入口处以导致45体积％至55体积％的所述氮氧化物为二氧化氮的量注入所述发动机废气中。
6.根据权利要求1所述的方法，其中在氧化催化剂的存在下，进行所述冷却的排放气体中的所述一氧化氮至二氧化氮的氧化。
7.根据权利要求1所述的方法，其中所述颗粒过滤器用在烧掉烟尘时有活性的催化剂催化。
8.在根据权利要求1所述的方法中使用的系统，在发动机废气通道内按顺序包括：
氧化催化剂单元，所述氧化催化剂单元用于将挥发性有机化合物和一氧化碳氧化为二氧化碳，并且将水和氮氧化物氧化为二氧化氮；
颗粒过滤器；
催化剂，所述催化剂用于选择性还原氮氧化物；
在用于选择性还原氮氧化物的所述催化剂上游的注入装置，所述注入装置用于将氨或尿素溶液注入所述发动机废气通道中；
在用于选择性还原氮氧化物的所述催化剂上游的注入装置，所述注入装置用于注入含有二氧化氮的排放气体；以及
在所述废气通道之外的氨氧化催化剂；以及
装置，所述装置用于从所述氨氧化催化剂冷却和氧化含有一氧化氮的排放气体，所述装置在其出口端处连接到用于注入含有二氧化氮的排放气体的所述注入装置。
9.根据权利要求8所述的系统，其中用于注入含有二氧化氮的排放气体的所述注入装置被布置在所述颗粒过滤器的上游。
10.根据权利要求8所述的系统，其中用于冷却和氧化含有一氧化氮的排放气体的所述装置为螺旋卷绕管的形式。
11.根据权利要求8所述的系统，其中用于冷却和氧化含有一氧化氮的排放气体的所述装置设置有氧化催化剂。
12.根据权利要求8所述的系统，其中所述颗粒过滤器用在烧掉烟尘时有活性的催化剂催化。
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