CN105715329A - 用于净化柴油发动机的排出气体的方法 - Google Patents

用于净化柴油发动机的排出气体的方法 Download PDF

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CN105715329A
CN105715329A CN201610083045.9A CN201610083045A CN105715329A CN 105715329 A CN105715329 A CN 105715329A CN 201610083045 A CN201610083045 A CN 201610083045A CN 105715329 A CN105715329 A CN 105715329A
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oxide
scr
catalyst
palladium
oxidation
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I.格卡斯
K.约汉森
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Umicore AG and Co KG
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Haldor Topsoe AS
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    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
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Abstract

本发明涉及用于净化柴油发动机的排出气体的方法，具体是提供一种用于在系统中净化柴油发动机的排出气体的方法，所述系统包括用于选择性催化还原的器件和优选地至少由催化层部分覆盖的柴油微粒滤器，所述柴油微粒滤器安装在用于选择性催化还原的器件的下游。用于催化氧化的器件安装在用于选择性催化还原的器件的上游和/或安装在用于选择性催化还原的器件与柴油微粒过滤器之间。用于喷射受控量的还原剂的器件安装在用于选择性催化还原的器件的入口，并且用于喷射受控量的烃类的器件安装在催化氧化器件的入口。

Description

用于净化柴油发动机的排出气体的方法
本申请是申请日为2009年12月16日、申请号为200980157185.4、发明名称为“用于净化柴油发动机的排出气体的方法”的发明专利申请的分案申请。
技术领域
本发明涉及来自柴油发动机的排出气体的净化。从排出气体中去除微粒、未完全燃烧的烃类、碳氧化物、CO以及氮氧化物、NOX。
本发明具体涉及一种净化方法，其包括用于过滤器再生的有效但简单的方法。
背景技术
用于排出气体净化的方法已经公知。US6863874中描述了一种方法，其中通过在过滤器之后进行氧化来去除排出气体中的杂质，其中烟灰被二氧化氮和氧气氧化。进一步在下游，将还原剂喷射进入NOX吸附器，并且随后安装三元催化剂或用于选择性还原的催化剂。
US6696031中公开了另一个过程，其中杂质是通过氧化、过滤以及选择性催化还原(SCR)来去除的。将氨喷射到氧化剂或SCR的上游并且进一步在该上游安装预氧化催化剂，烃类可被引入所述预氧化催化剂中。计算机必须控制这两股氨流。
通过US6871489的方法使气体穿过氧化催化剂、配备旁通装置的冷却器、包括尿素喷射的SCR部分、穿过加热器并最后穿过柴油微粒过滤器来去除来自排出气体的杂质。以此方式，必须通过提高过滤器的温度使过滤器再生，所述过滤器温度的提高通过增加来自加热器的热量输出来实现。
这些过程不仅复杂、耗能或具有低的尿素分解速度，同时在发动机冷起动时具有缓慢的NOX催化还原作用。
发明内容
本发明的总体目的是提供一种净化过程，所述净化过程有效地去除来自排出气体的颗粒、未完全燃烧的烃类、碳氧化物、CO和氮氧化物、NOX并且再生过滤器，同时又非常简单。
本发明提供一种用于在系统中净化柴油发动机的排出气体的方法，所述系统包括用于选择性催化还原的器件以及柴油微粒过滤器，所述柴油微粒过滤器优选地至少由催化层部分覆盖并且安装在用于选择性催化还原的器件的下游。用于催化氧化的器件安装在用于选择性催化还原的器件的上游和/或安装在用于选择性催化还原的器件与催化柴油微粒过滤器之间。用于喷射受控量的还原剂的器件安装在用于选择性催化还原的器件的入口，并且用于喷射受控量的烃类的器件安装在催化氧化器件的入口。
本发明提供如下配置：催化柴油微粒过滤器通过关闭还原剂喷射而被动再生，并且催化柴油微粒过滤器通过打开至少一个用于催化氧化的器件的烃类入口喷射以及可选地关闭还原剂喷射而主动再生。过滤器在高达500℃的温度下通过NO2被动再生，并且在500℃至700℃的温度下主动再生。
还原剂是氨、氨的水溶液、尿素、尿素的水溶液、三聚氰酸。其他潜在的氮基反应剂包括氰尿酰胺、三聚氰酸二酰胺（ammelinge）、氰酸氨、双缩尿素、氨基甲酸铵、碳酸氨、甲酸氨、三聚氰胺以及三氰基尿素（tricyanourea）。氨、氨的水溶液、尿素、尿素的水溶液、三聚氰酸是更优选的。
烃类是燃料，优选地是柴油发动机的燃料。在钒基催化剂或沸石基催化剂或功能性酸性基底金属氧化混合物存在的情况下发生选择性催化还原。钒基催化剂是可能添加有钨或钼氧化物的钛氧化物上的钒氧化物。沸石基催化剂包括铜和/或铁改变的β沸石、ZSM-5或菱沸石，而功能性酸性基底金属氧化混合物包括酸性的铈锆氧化混合物和锆钛氧化混合物。在从150℃至550℃的温度下使用钒催化剂，而从150℃至800℃的温度下使用沸石基催化剂或酸性基底金属混合物催化剂。
当第一氧化催化剂安装在选择性催化还原器件的上游并且第二氧化催化剂安装在选择性催化还原器件与柴油微粒过滤器之间时，随后可将氨喷射进入第一氧化催化剂。第一氧化催化剂包括镧氧化物促进的铝氧化物上的铂和钯、或硅氧化物促进的钛氧化物上的铂和钯、或锆氧化物促进的铈氧化物上的铂和钯。第二氧化催化剂包括镧氧化物促进的铝氧化物上的钯、或硅氧化物促进的钛氧化物上的钯、或锆氧化物促进的铈氧化物上的钯、或者铜和锰氧化物的混合物或铜和锰氧化物的混合物上的钯。
柴油微粒过滤器上的催化层包括可能与贵金属-如钯和铂组合的基底金属氧化物的混合物。在EP1916029中描述了具有在铈氧化物与锆氧化物的混合物上的钯的特别有利的示例。
测量穿过过滤器的压降，并且所产生的信号用于控制还原剂的添加和燃料的添加。
本发明还包括用于执行上述方法的系统。
这种系统保证了选择性还原催化作用的快速冷起动，并且获得了很高的NOX转化率。通过还原剂和烃类喷射的主动开/关管理，保证了催化过滤器的被动和主动再生。
本发明在净化柴油发动机的排出气体方面非常有用，所述柴油发动机安装在机动交通工具中，所述机动交通工具通常为客车、货车、卡车以及船舶。此外，在由柴油发动机驱动的动力设备中，本发明的过程可以有利地净化排出气体。
附图说明
图1是根据公知技术的排出气体净化过程的示意图；
图2是根据本发明的过程的一个优选实施方式的排出气体净化过程的示意图；
图3是根据本发明的过程的另一个优选实施方式的排出气体净化过程的示意图；
图4是根据本发明的过程的再一个优选实施方式的排出气体净化过程的示意图；和
图5和图6示出了cDPF上的压降的测量值的曲线图。
具体实施方式
柴油发动机以过量空气运转，并且柴油发动机的排出气体包括氮氧化物、NOX、一氧化碳、CO、微粒物质以及不完全燃烧的烃类，这些都对健康有威胁。
本发明在排出气体的正常净化期间基本包括三个过程：
催化氧化作用，其中
CO、NO和HC与O2反应以生成CO2、NO2和H2O以及热量；
选择性氧化还原作用，其中
NO和NO2通常被NH3还原从而生成N2和H2O；
并且在催化性涂层的过滤器中捕获颗粒，其中
CO、C、HC和NH3的可能的滑移部分被氧化生成N2、CO2和H2O；
此处C是指沉积在柴油微粒过滤器上的微粒物质或烟灰。
然而当微粒堆积在过滤器上时，过滤器可通过与二氧化氮、过滤器涂层的基底金属氧化物氧化来再生，或在更高的温度下与排出气体中的氧气氧化来再生：
C和HC被NO、NO2和/或O2氧化以生成N2、CO2和H2O。
当前应用的柴油机排气系统技术（公知技术）的特征是具有如图1所示催化过滤器下游的SCR催化剂。
排出气体1从发动机流向氧化催化剂2，然后被氧化的排出气体3输送至柴油微粒过滤器4。在将该还原剂5喷射到排出气体之后，随后混合排出气体6被引入到催化剂7以用于选择性催化还原SCR，来自SCR的清洁排出气体8离开催化剂7。当需要提高温度时，将烃类9之后喷射到发动机中或将烃类9在发动机与氧化催化剂2之间喷射到排出气体1中。在下面的过程（1）中将对此进一步描述：
（1）发动机→DOC→cDPF→Ureainj→zSCR
其中DOC是含有用于NO2生成的Pt的柴油氧化催化剂，并且cDPF是催化性的烟灰过滤器，所述过滤器也可含有用于NO2生成的Pt。
Ureainj是喷射的还原剂，典型的是尿素的水溶液，zSCR是沸石基SCR催化剂或功能性的酸性基底金属氧化混合物。
在具有大约600℃的过滤器入口温度的过滤器的强制再生期间，系统将按照如下过程操作：
（2）发动机→HCinj→DOC→cDPF→zSCR
其中HCinj是烃类，所述烃类从发动机且在DOC上游喷射入排出气体。
用NO2进行的烟灰的被动再生在过程（1）所示构造中进行。
这种系统具有若干缺点。加热和从冷起动的SCR反应的起动比较慢，并且也在测试周期测得的总NOX排放将比较高。因为尿素喷射需要最低温度为200℃，所以该起动也较慢。进一步地，zSCR催化剂应能够承受至少750℃的过滤器再生温度，并且用zSCR进行的操作通常需要受控的NO2/NO比率，所述比率受到cDPF的干扰，因为微粒物质也与过滤器中的NO2反应。最后，所述系统非常昂贵。
图2示出了本发明的优选实施方式。来自发动机的排出气体1穿过氧化催化剂2、用于选择性催化还原的催化剂7，并且作为最后一步通过柴油微粒过滤器4。将还原剂5喷射到氧化催化剂2与SCR催化剂7之间。可将烃类9喷射到氧化催化剂2的上游。
在下面的过程（3）中将进一步描述新的柴油机排气系统，所述柴油机排气系统具有反向构造，SCR在cDPF之前。所述柴油机排气系统还包括一种新的特殊的管理。
（3）发动机→DOC→Ureainj→zSCR→cDPF
其中zSCR是沸石基SCR催化剂或功能性的酸性基底金属氧化混合物，所述zSCR能忍受最低750℃的温度。
cDPF是优选地具有催化性涂层的柴油微粒过滤器。在这种实施方式中，特别有利的是，用钯基金属氧化物涂层-如可从HaldorTopsФeA/S商购并且在专利申请EP1916029中描述的BMC-211催化剂。这种催化剂限制可能的NO2排放并且便于烟灰在300-600℃的温度范围内燃烧。
DOC是可具有不同成分的柴油机氧化催化剂。这种催化剂是在促进型金属氧化物载体上的贵金属，所述贵金属通常施加到单块框架衬底-如堇青石、碳化硅、多铝红柱石或费克拉洛伊合金（Fecralloy）。它通常含有铂。它包括在镧氧化物促进的铝氧化物上的铂和钯，或在硅氧化物促进的钛氧化物上的铂和钯，或在锆氧化物促进的铈氧化物上的铂和钯。
本发明将在柴油机排气系统中的被动和主动状态下保证过滤器烟灰有效地再生，其中SCR催化剂放置在cDPF的上游。本发明还保证冷起动时的高NOX转换率。在主动再生期间，烟灰与排出气体中的O2的燃烧在575℃以上的温度范围中进行。被动NO2再生-即烟灰使用NO2燃烧可在250-大约450℃的温度范围中进行。最后，被动催化剂烟灰燃烧也可在催化过滤器中进行。在300-600℃的温度间隔中，基底金属催化剂BMC-211可有助于烟灰燃烧。
如下面的过程（4）所示，在发动机中进行柴油后喷射（dieselpostinjection）的情况下，通过同时停止尿素喷射，以大约620℃的过滤器入口温度进行系统（3）中的主动再生。在这种系统中，需要SCR催化剂-例如沸石SCR催化剂可承受此温度：
（4）发动机→HCinj→DOC→zSCR→cDPFTfilterin=620℃达10分钟。
过程（3）与现有技术相比较具有许多优点，但是在通过二氧化氮进行被动过滤器再生期间似乎具有一个缺点。本发明解决了系统（3）的这种可能的缺点，所述缺点是指与具有如公知技术过程（1）中所示的催化过滤器下游的SCR催化剂的系统相比，系统（3）具有SCR下游的非常低浓度的NO2。本发明确保用NO2的烟灰过滤器的被动再生。
本发明还涉及系统（3）或（4）的主动管理。本发明包括通过停止尿素喷射NO2浓度在短时间间隔内暂时增加，所以NO2生成以用于被动再生并且可节省柴油燃料。当穿过催化过滤器的压降增加至预定值并且过滤器入口温度达到预定值-至少应为250℃时，这种暂时的NO2增加被起动。然后系统（3）将如系统过程（5）所示进行操作。
（5）发动机→DOC→zSCR→cDPF
在大约300-400℃的温度范围中，NO2/NO对于高NO2容量将是最佳的。通过如下面的过程（6）所示暂时关闭发动机排气再循环（EGR)同时如过程（5）所示停止尿素喷射，NO2浓度和被动烟灰燃烧的效果可进一步增加：
（6）发动机（无EGR)→DOC→zSCR→cDPF。
系统（3）进一步的改进可通过代替尿素的氨（NH3)的喷射来实现，原系统需要热量以用于水蒸发和尿素分解。然后SCR反应可从大约150℃开始，并且可将SCR催化剂放置成与柴油机氧化催化剂DOC更接近，因为NH3混合可在几厘米排气管长度f.-如5厘米内进行。
并且当通过任何政府标准测试周期进行测试时，可在道路上实现较低的NOx排出所述排气系统。
由过程(5）和(6)示出通过停止NH3喷射而改善的系统被动再生。
系统（5）的进一步可能的改进是喷射氨（NH3)到DOC的上游。通过这样做，在DOC中生成额外的NO2并用于被动再生。与此同时，系统中的温度增加。下面示出了用于具有和不具有排气再循环的所述过程。
（7）发动机→NH3inj→DOC→zSCR→cDPF
（8）发动机（无EGR)→NH3inj→DOC→zSCR→cDPF
系统（3）对于具有柴油后喷射选项的客车具有特殊的重要性。
图3中示出了本发明的另一个优选的实施方式，其中示出了来自发动机的排出气体1连续穿过第一氧化催化剂2、选择性还原催化剂7、第二氧化催化剂10以及最后的柴油微粒过滤器4。烃类9和11可被加入到第一氧化催化剂2和第二氧化催化剂10上游的排出气体流，同时还原剂5被喷射入选择性还原催化剂7。从过滤器4流出的是清洁的排出气流8。
还原剂5的量由阀12控制。所述阀12将接收来自f.inst.的信号-穿过过滤器4的压力差测量值，而阀12将关闭以便起动被动再生。类似地，当需要增加氧化催化剂2、10中的一个的入口或出口温度时，阀16和/或14将打开。可在此选择性地增加氨。下面将进一步描述该实施方式。正常操作被描述为：
（9）发动机→DOC（1）→Ureainj→SCR→HCinj→DOC（2）→cDPF。
这是重要的示例且被称为HaldorTopsФe反向标准系统-EuroVI系统。SCR可以是钒基SCR或沸石SCR或功能性酸性基底金属氧化混合物。在主动再生期间，该过程为：
（10）发动机→DOC（1）→NH3inj→zSCR→HCinj→DOC（2）→cDPF。
而在冷起动且同时具有主动再生时：
（11）发动机→NH3inj→DOC（1）→NH3inj→zSCR→HCinj→DOC（2）→cDPF。
通过将NH3喷射到第一上游DOC（1），冷起动性能可通过产生的热量而改进，并且NO2/NO比率对zSCR上的zSCR反应而言也将变得更佳。
DOC（1）是针对系统（3）描述的DOC。
DOC（2）催化剂是促进型金属氧化物载体上的贵金属，所述贵金属通常施加到单块框架衬底-例如堇青石、碳化硅富铝红柱石或费克拉洛伊合金（Fecralloy）上。这种催化剂也可以是具有或不具有贵金属的基底金属氧化物的混合物，所述贵金属通常施加到单块框架衬底-例如堇青石、碳化硅富铝红柱石或费克拉洛伊合金（Fecralloy）上。它通常不包含铂。它包含镧氧化物促进的铝氧化物上的钯、或硅促进的钛氧化物上的钯氧化物、或锆氧化物促进的铈氧化物上的钯或者铜和锰氧化物的混合物或铜和锰氧化物的混合物上的钯。
系统（9）有利于卡车和客车应用。图4示出了第三个优选实施方式。在此，来自发动机的排出气体1穿过选择性催化还原剂7、催化氧化剂10并最终穿过过滤器4。添加了还原剂5到排出气体1，且烃类11可添加到选择性催化还原剂7与催化氧化剂10之间。
这种排气系统的优点是，至SCR催化剂的最高入口温度可与发动机出口温度相同-大约是550℃。这种系统将有助于选择标准钒基SCR催化剂（V-SCR）。通过V-SCR的使用，该过程将为下列型式:
（12）发动机→Ureainj→V-SCR→HCinj→DOC→cDPF
铜基沸石SCR催化剂Cu-zSCR可用作选定的SCR催化剂，因为它较少依赖于NO2/NO比率，但它需要是Cu-zSCR类型的，所述Cu-zSCR类型能忍受从发动机排放的HC。
所述系统具有NH3喷射而非尿素以用于SCR反应并且同时具有主动再生，所述系统将为下列型式：
（13）发动机→NH3inj→V-SCR→HCinj→DOC→cDPF
在系统（13）中，从发动机歧管至V-SCR催化剂的距离可通过因数10而减少-从50cm减至5cm。所以，在冷起动时，发动机热量不被用于加热多余的管道长度而是用于化学反应的起动。在受控的被动再生期间-此时停止NH3喷射，系统（13）将暂时为下列型式：
（14）发动机→V-SCR→DOC→cDPF
并且等同的无EGR型式为：
（15）发动机（无EGR)→V-SCR→DOC→cDPF
系统（12）对于卡车应用特别有利。
示例1
在间歇性尿素定量配料以及暂时高NO2容量的情况下进行7个世界协调测试循环（worldharmonizedtestcycle）之后，在具有SCR+DOC+cDPF系统的Scania12升发动机上进行的发动机测试台架实验显示：烟灰负载压降没有改变。
cDPF上的压降的测量值用于某天测得的第1和第7个重复的世界协调测试循环（WHTC），其中所述系统以低和高的尿素定量配料被管理。
在图5中两条曲线是相同的，因此它们写在彼此的顶端。这意味着，没有看到额外烟灰负载引起的压降增加。这种结果将与下面的参照示例进行比较。
在该参照示例中，对于高速SCR反应尿素定量配料是持续的并且大量的。这就提供了较低的NO2和NOx（大约1-2gNOx/KWh）流出SCR催化剂-进入cDPF。在图6中，我们看到与图5相反，上面的压降从第1WHTC循环增加至第7循环。这意味着，烟灰在过滤器上积聚。

Claims (14)

1.一种用于在系统中净化柴油发动机的排出气体的方法，所述系统包括：
用于选择性催化还原的器件；
柴油微粒过滤器，所述柴油微粒过滤器优选地至少由催化层部分覆盖并且安装在用于选择性催化还原的器件的下游；
用于催化氧化的器件，所述用于催化氧化的器件安装在用于选择性催化还原的器件的上游和/或安装在用于选择性催化还原的器件与柴油微粒过滤器之间；
用于喷射受控量的还原剂的器件，所述还原剂被喷射到用于选择性催化还原的器件的入口；以及
用于喷射受控量的烃类的器件，所述烃类被喷射到用于催化氧化的器件的入口；
其特征在于，所述柴油微粒过滤器通过关闭还原剂的喷射而被动再生；并且所述柴油微粒过滤器通过打开至少一个用于催化氧化的器件的烃类入口喷射以及可选地关闭所述还原剂的喷射而主动再生。
2.如权利要求1所述的方法，其中所述过滤器在高达500℃的温度下通过NO2被动再生。
3.如权利要求1所述的方法，其中所述过滤器在从500℃至700℃的温度下主动再生。
4.如权利要求1所述的方法，其中所述还原剂是氨、氨的水溶液、尿素、尿素的水溶液、三聚氰酸、氰尿酰胺、三聚氰酸二酰胺、氰酸氨、双缩尿素、氨基甲酸铵、碳酸氨、甲酸氨、三聚氰胺或三氰基尿素。
5.如权利要求4所述的方法，其中所述还原剂是氨、氨的水溶液、尿素、尿素的水溶液或三聚氰酸。
6.如权利要求1所述的方法，其中所述烃类是燃料，优选地是与柴油发动机的燃料相同的燃料。
7.如权利要求1所述的方法，其中所述选择性催化还原于存在钒基催化剂或沸石基催化剂或功能性酸性基底金属混合氧化催化剂的情况下发生。
8.如权利要求7所述的方法，其中所述钒基催化剂是可能添加了钨或钼氧化物的钛氧化物上的钒氧化物，所述沸石基催化剂是铜和/或铁改变的β沸石、ZSM-5或菱沸石，而功能性酸性基底金属混合氧化催化剂包括酸性铈锆氧化混合物和锆钛氧化混合物。
9.如权利要求7所述的方法，其中所述钒基催化剂在从150℃至550℃的温度下使用，而所述沸石基催化剂在从150℃至800℃的温度下使用。
10.如权利要求1所述的方法，其中所述柴油微粒过滤器上的催化层包括贵金属-优选是钯和铂可选地与基底金属氧化物组合的混合物。
11.如权利要求1所述的方法，其中第一氧化催化剂安装在选择性催化还原器件的上游，并且第二氧化催化剂安装在选择性催化还原器件与柴油微粒过滤器之间，而氨被喷射进入所述第一氧化催化剂。
12.如权利要求1所述的方法，其中安装在用于选择性催化还原的器件的上游的所述用于催化氧化的器件包括催化剂，所述催化剂包括镧氧化物促进的铝氧化物上的铂和钯或硅氧化物促进的钛氧化物上的铂和钯或锆氧化物促进的铈氧化物上的铂和钯；并且安装在用于选择性催化还原的器件的下游的所述用于催化氧化的器件包括催化剂，所述催化剂包括镧氧化物促进的铝氧化物上的钯或硅氧化物促进的钛氧化物上的钯或锆氧化物促进的铈氧化物上的钯或者铜和锰氧化物的混合物或铜和锰氧化物的混合物上的钯。
13.如权利要求1所述的过程，其中穿过过滤器的压降被测量，并且所产生的信号用于控制还原剂的添加和烃类的添加。
14.一种使用根据权利要求1-13所述的方法的系统。
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