CN102441328A - 包括铂族金属捕集装置的柴油发动机废气处理系统和方法 - Google Patents

包括铂族金属捕集装置的柴油发动机废气处理系统和方法 Download PDF

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CN102441328A
CN102441328A CN2011103083943A CN201110308394A CN102441328A CN 102441328 A CN102441328 A CN 102441328A CN 2011103083943 A CN2011103083943 A CN 2011103083943A CN 201110308394 A CN201110308394 A CN 201110308394A CN 102441328 A CN102441328 A CN 102441328A
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CN102441328B (zh
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H·詹
G·卡瓦塔欧
J·W·吉拉德
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Abstract

本发明提供一种包括位于柴油机氧化催化剂和SCR催化剂之间的铂族金属捕集装置的柴油发动机废气处理系统和方法。所述铂族金属捕集装置捕集在发动机运行过程中可从柴油机氧化催化剂释放的痕量铂族金属，并防止所述痕量铂族金属在SCR催化剂上积聚，从而防止SCR催化剂的潜在污染以及确保SCR催化剂的性能不被抑制。

Description

包括铂族金属捕集装置的柴油发动机废气处理系统和方法
技术领域
本文所述的实施例涉及柴油发动机废气处理系统和方法，更特别地涉及利用铂族金属捕集装置以防止SCR催化剂的污染的废气处理系统和方法。
背景技术
柴油发动机废气处理系统已知用于将诸如氧化氮(NOx)的气体排放物转化为环境可接受的化合物。这种系统通常包括柴油机氧化催化剂(DOC)、选择性催化还原催化剂(SCR)，以及柴油机微粒过滤器(DPF)。
柴油机氧化催化剂位于柴油发动机的废气流中，并通常含有铂族金属(PGM)、贱金属或它们的组合。这些催化剂促进CO和HC排放物转化为二氧化碳和水。
选择性催化还原催化剂(SCR)用于将NOx转化为N2，并通常包含贱金属且利用通常为水性尿素形式的氨还原剂，所述氨还原剂在柴油机氧化催化剂的下游被注入废气流。在水蒸发和尿素水解之后，形成的氨与在SCR催化剂上的废气流中的NOx反应以形成N2。
柴油机微粒过滤器(DPF)从发动机废气中收集烟灰或微粒物质。通常将选自铂族金属的贵金属催化剂涂布于DPF上以用于去除CO、HC和NH3漏失。
已观察到包括涂布有铂族金属的柴油机氧化催化剂的处理系统在某些条件(如高温操作)下会损失痕量的铂或其他铂族金属。来自DOC的痕量铂族金属升华，并随后在位于DOC下游的SCR催化剂上积聚，使得SCR催化剂的功能被抑制。这是由于用于氨氧化的铂族金属的高活性导致极少或者没有氨可用于SCR反应。此外，由于铂族金属催化剂使得氨生成NOx和N2O，因此当由于铂族金属中毒而导致SCR被抑制时，实际上会产生NOx水平的增加。已发现低至0.0005重量％的铂水平可对SCR性能产生显著影响。参见Jagner等人的“Detection，Origin，and Effect of Ultra-LowPlatinum Contamination on Diesel-SCR Catalysts，”SAE International PaperNo.2008-01-2488，(2008)。
因此，本领域需要一种防止铂族金属沉积在位于柴油机氧化催化剂下游的SCR上的柴油发动机废气系统，且需要一种有效实现燃烧组分的转化和废气中微粒的去除的系统。
发明内容
本发明的实施例通过提供一种包括位于柴油机氧化催化剂下游的铂族金属捕集器的柴油发动机废气处理系统和方法而满足了那些需要。所述铂族金属捕集器起到了捕集从柴油机氧化催化剂释放的痕量铂族金属的作用，以防止所述金属沉积在位于柴油机氧化催化剂下游的SCR催化剂上。
根据一个方面，提供了一种柴油机废气处理系统，其包括含有位于废气流中的铂族金属的柴油机氧化催化剂、位于柴油机氧化催化剂下游并捕集从柴油机氧化催化剂释放的铂族金属的铂族金属捕集器，以及位于铂族金属捕集器下游的选择性还原催化剂(SCR)。
所述柴油机氧化催化剂优选包含铂和钯的组合。所述SCR催化剂优选包含沸石和选自铜和铁的贱金属。
在一个实施例中，所述铂族金属捕集器包括氧化铈。在另一实施例中，所述铂族金属捕集器包括钙钛矿材料。所述钙钛矿材料优选包含CaTiO3。
所述处理系统优选还包括柴油机微粒过滤器，所述柴油机微粒过滤器可位于SCR催化剂的下游、铂族金属捕集器的下游，或铂族金属捕集器的上游。
在另一实施例中，所述处理系统还包括贫NOx捕集器，所述贫NOx捕集器可位于铂族金属捕集器的上游或下游。
所述处理系统优选还包括用于将氨源或尿素源提供至废气流的还原剂传递系统。所述还原剂传递系统优选直接位于SCR催化剂的上游。
在另一实施例中，提供了一种处理柴油发动机废气的方法，在所述方法中使废气通过废气处理系统，所述废气处理系统包括位于柴油机氧化催化剂和SCR催化剂之间的铂族金属捕集器，相比于不包括铂族金属捕集器的废气系统，所述铂族金属捕集器减少SCR催化剂上的铂族金属污染物。所述方法优选包括将氨源或尿素源提供至废气流。
因此，本发明的实施例的一个特征在于提供了一种柴油机废气处理系统和方法，其利用铂族金属捕集器以捕集从柴油机氧化催化剂释放的铂族金属，从而防止SCR催化剂的污染。
本发明的其他特征和优点将通过如下描述、如下附图和所附权利要求书而显而易见。
附图说明
图1为根据本发明的一个实施例的柴油发动机废气处理系统的示意图；
图2为包括贫NOx捕集器和柴油机微粒过滤器的本发明的另一实施例的示意图；
图3为本发明的另一实施例的示意图；
图4为本发明的另一实施例的示意图；
图5为本发明的另一实施例的示意图；以及
图6为本发明的另一实施例的示意图。
具体实施方式
在一个优选的实施例中，提供了一种废气处理系统，其包括位于柴油机氧化催化剂和SCR催化剂之间的铂族金属捕集器。所述系统降低了SCR催化剂污染的可能性，使得SCR催化剂的性能不被抑制。因此，当相比于不包括捕集器的废气处理系统时，包括铂族金属捕集器的系统降低了铂族金属污染，同时仍然提供NOx的有效去除。
铂族金属捕集装置可包括涂布有含铈氧化物(以约30至300g/L的载荷)的块体(monolith)。尽管不希望受限于任何特定的工作原理，据信氧化铈与铂的强相互作用促进了从上游DOC升华/释放的铂族金属的捕集。
或者，所述铂族金属捕集装置可包括具有式ABO3的钙钛矿材料，其中A-B包括但不限于Ca+2-Ti+4、Ba+2-Ti+4、Ln+3-Co+3或La+3-Fe+3。具有相对较高表面积的钙钛矿材料可使用相应的金属醇盐通过溶胶-凝胶法制得。钙钛矿材料优选包括CaTiO3，其可通过以1∶1的Ca/Ti比组合硝酸钙(Ca(NO3)2)和钛酸四异丙酯(Ti(i-C3H7O)4)而制得。例如，可将硝酸钙和钛酸四异丙酯溶解于2-甲氧基乙醇中，并可加入少量硝酸以形成前体溶液，所述前体溶液随后被干燥，在约400℃下热解，然后在约600至800℃下在空气中加热。
或者，可通过如下方法制得CaTiO3：将Ca(NO3)2与乙醇、水和HNO3组合以形成溶液。将该溶液逐滴加入到Ti(i-C3H7O)4和乙醇的溶液(以1∶1的Ca/Ti比)中。可在200℃下将所述溶液蒸发至干燥粉末，然后在约600℃下煅烧。这些方法制得粒径为约22至50nm的CaTiO3粉末。
可使用含有钙钛矿细粉的浆状溶液将CaTiO3钙钛矿材料涂布于蜂窝状基材上。所述浆状溶液可任选地含有氧化铝、氧化锆(ZrO2)、氧化铈(CeO2)，和Ce-Zr混合氧化物(CexZr1-xO2)中的一种或多种。所述涂层载荷可为约50至约350g/L。
涂布CaTiO3的基材起到捕集可从柴油机氧化催化剂释放的升华的贵金属的作用。此外，尽管不希望受限于任何特定的工作原理，据信从DOC释放的痕量铂族金属被捕集于材料的晶格结构中。
现在参见图1，其显示了柴油机废气处理系统10的一个实施例。如以其最简化形式所示，所述废气处理系统被连接至柴油发动机的排气歧管12，并包括位于SCR催化剂18的上游的柴油机氧化催化剂14。所述系统包括位于DOC和SCR催化剂之间的铂族金属捕集器16。
所述柴油机氧化催化剂14以约30至约300g/L的载荷被涂布于耐火无机氧化物或陶瓷蜂窝状基材上作为涂层，并利用选自铂、钯或其组合的催化剂材料，且也可含有沸石。所述涂层还可包含粘合剂，如氧化铝、二氧化硅、氧化钛或氧化锆。
所述SCR催化剂18包含沸石和选自铜和铁的贱金属。SCR催化剂涂层以约30至约300g/L的载荷进行涂布，并可通过用含有贱金属、沸石和粘合剂材料(如氧化铝、二氧化硅、氧化钛或氧化锆)的浆料涂布多孔惰性基材而制得。或者，贱金属/沸石可与陶瓷粘合剂/纤维组合并挤出成为块体。
再次参见图1，所述处理系统优选还包括还原剂传递系统20，所述还原剂传递系统20与直接在SCR催化剂18上游的排气歧管连接。还原剂(如氨、水性尿素或其他产氨化合物)被储存于储存容器(未显示)中，并通常以还原剂和水的汽化混合物的形式以计量量传递至还原剂传递系统。所述还原剂传递系统包括注射器22，所述注射器22用于在适当时间将适当量的还原剂注入废气流。
在示于图2的本发明的另一实施例中，所述废气处理系统还可任选地包括位于DOC14下游的贫NOx捕集器(LNT)26以协助废气中的NOx的进一步还原。LNT26包含一种或多种铂族金属，并优选包含铂、钯和铑的混合物。优选地，所述贫NOx捕集器具有约30至约300g/ft3之间的贵金属载荷。所述贫NOx捕集器还包含选自一种或多种碱金属或碱土金属的NOx吸附材料。
应了解的是，在包括贫NOx捕集器的实施例中，由于贫NOx捕集器在其运行过程中产生氨，因此还原剂传递系统的使用是任选的。
还如图2所示，所述废气处理系统还可包括在SCR催化剂下游的柴油机微粒过滤器28以用于收集烟灰和微粒物质。所述柴油机微粒过滤器优选为壁流式过滤器，其包括孔隙率为约30至80％的高度多孔过滤器基材。孔隙的尺寸优选为约10至50μm。应了解孔径分布可在整个过滤器基材内变化。
合适的过滤器基材包括耐火无机氧化物或陶瓷或金属材料，如堇青石、富铝红柱石、碳化硅、钛酸铝、α-氧化铝、二氧化硅，以及磷酸锆碱金属和碱土金属(NZP)。
在示于图3的另一实施例中，可设置柴油机微粒过滤器28和LNT26的位置使得DPF28直接位于DOC催化剂14的下游，且LNT26直接位于柴油机微粒过滤器28的下游。在示于图4的又一实施例中，LNT和DPF的位置颠倒。
在示于图5的又一实施例中，所述系统包括位于铂族金属捕集器16和SCR催化剂18之间的柴油机微粒过滤器28。
在示于图6的又一实施例中，所述柴油机微粒过滤器28位于DOC14和捕集装置16之间，且LNT26位于捕集装置16和SCR催化剂18之间。
再次参见图1，在运行过程中，当由柴油发动机(未显示)产生的废气通过排气歧管12时，所述废气经过柴油机氧化催化剂14以发生未燃烧的HC和CO向H2O和CO2的转化。所述废气随后流过铂族金属捕集装置，之后流过SCR催化剂。所述废气随后流向废气出口(未显示)。
当气体经过SCR催化剂18时，所述催化剂通过使用自还原剂传递系统20提供的氨源的选择性催化还原而从气流去除NOx。通常，还原剂传递系统20利用液体尿素/水溶液，所述液体尿素/水溶液以计量的间隔从DOC催化剂14的下游注入。注入的液体尿素/水混合物蒸发并水解形成氨。因此，通过使用氨的NOx的选择性催化还原，气体中的NOx组分被转化而形成氮气。
已参考本发明的优选实施例详细描述了本发明，明显的是在不脱离本发明的范围下可能进行修改和变化。

Claims (20)

1.一种柴油机废气处理系统，其包括：
包含位于废气流中的铂族金属的柴油机氧化催化剂；
位于所述柴油机氧化催化剂下游、并适于捕集从所述柴油机氧化催化剂释放的铂族金属的铂族金属捕集器；以及
位于所述铂族金属捕集器下游的选择性还原催化剂(SCR)。
2.根据权利要求1所述的处理系统，其中所述铂族金属捕集器包括氧化铈。
3.根据权利要求1所述的处理系统，其中所述铂族金属捕集器包括钙钛矿材料。
4.根据权利要求3所述的处理系统，其中所述钙钛矿材料包含CaTiO3。
5.根据权利要求1所述的处理系统，其包括位于所述SCR催化剂下游的柴油机微粒过滤器。
6.根据权利要求1所述的处理系统，其包括位于所述铂族金属捕集器下游的柴油机微粒过滤器。
7.根据权利要求1所述的处理系统，其包括位于所述铂族金属捕集器上游的柴油机微粒过滤器。
8.根据权利要求1所述的处理系统，其包括位于所述铂族金属捕集器上游的贫NOx捕集器。
9.根据权利要求1所述的处理系统，其包括位于所述铂族金属捕集器下游的贫NOx捕集器。
10.根据权利要求1所述的处理系统，其包括用于将氨源或尿素源提供至所述废气流的还原剂传递系统。
11.根据权利要求10所述的处理系统，其中所述还原剂传递系统直接位于所述SCR催化剂的上游。
12.根据权利要求1所述的处理系统，其中所述SCR催化剂包含沸石和选自铜和铁的贱金属。
13.根据权利要求1所述的处理系统，其中所述柴油机氧化催化剂包含铂和钯的组合。
14.一种用于处理柴油发动机废气的方法，其包括：
提供一种废气处理系统，所述废气处理系统包括：由位于废气流中的铂族金属组成的柴油机氧化催化剂；位于所述柴油机氧化催化剂下游、并适于捕集从所述柴油机氧化催化剂释放的铂族金属的铂族金属捕集器；和位于所述铂族金属捕集器下游的选择性还原催化剂(SCR)；以及
使废气通过所述废气处理系统；其中相比于不包括铂族金属捕集器的废气系统，所述铂族金属捕集器减少在所述SCR催化剂上的铂污染物。
15.根据权利要求14所述的方法，其中所述铂族金属捕集器包括氧化铈。
16.根据权利要求14所述的方法，其中所述铂族金属捕集器包括CaTiO3。
17.根据权利要求14所述的方法，其包括将氨源或尿素源提供至所述废气流。
18.根据权利要求14所述的方法，其中所述处理系统包括位于所述SCR催化剂下游的柴油机微粒过滤器。
19.根据权利要求14所述的方法，其中所述处理系统包括位于所述铂族金属捕集器上游或下游的柴油机微粒过滤器。
20.根据权利要求14所述的方法，其中所述处理系统还包括位于所述铂族金属捕集器上游或下游的贫NOx捕集器。
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