CN100351502C - 降低柴油机排出物的方法 - Google Patents

降低柴油机排出物的方法 Download PDF

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CN100351502C
CN100351502C CNB988051605A CN98805160A CN100351502C CN 100351502 C CN100351502 C CN 100351502C CN B988051605 A CNB988051605 A CN B988051605A CN 98805160 A CN98805160 A CN 98805160A CN 100351502 C CN100351502 C CN 100351502C
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杰里米·D·彼得-霍布林
詹姆斯·M·瓦伦丁
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Clean Diesel Technologies Inc
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Abstract

能使柴油机在低颗粒物排放下进行运行。柴油机装有铂催化的颗粒物收集器。柴油机在柴油机燃料和燃料可溶性铈组合物的混合物下运行以便随铈含量的降低而降低收集器的平衡点。优选的是，燃料还含有燃料可溶性有机铂族金属化合物，或把有效的铂族金属化合物加到废气中或燃烧空气中。

Description

降低柴油机排出物的方法
技术领域
本发明涉及可以使柴油机在有效地降低颗粒物和NOX排放下进行运行的方法。
用于柴油机的颗粒物收集器已很普遍，这是因为NOX和颗粒物之间存在着固有的权衡所造成的，当采取措施以降低其中之一时，另一种就增加。从原理上讲，用收集器通过一些技术，如废气循环、发动机定时调节或其他的已知技术，能使NOX降低到很低的程度。但是，当经过收集器的压降过高时，由于发动机效率的损失，用收集器捕集颗粒物就成为问题。
就现行技术而言，迅速积累的颗粒物在实际情况下并不能减少。催化的收集器，虽实际上有助于颗粒物的燃烧，但低温，倾向于过快地失活，使其成为经济上待解决的问题。同样，燃料添加剂也不能完全解决问题。
发明内容
本发明的第一个目的是提供一种方法，该法能使柴油机通过降低平衡点(稳定烧尽温度)而使用颗粒物收集器，以使收集器达到实际上低而持续的水平。
本发明第二个目的是提供一种方法，该法能优化柴油机的运行，在处理颗粒物，例如PM2.5的同时使NOX减少。
本发明第三个目的是提供一种用较少的燃料添加剂，例如较以前更有效的铈以无源再生颗粒物收集器的方法。
本发明第四个目的是提供一种能同时降低由柴油机排放的颗粒物，未燃料烃以及一氧化碳的方法。
本发明第五个目的是提供一种能弥补通常与柴油机颗粒物收集器有关的燃料经济上的损失的方法。
本发明第六个目的是提供一种特用添加剂，该添加剂以合适的配比加到柴油机燃料中以再生已失效的催化收集器的活性。
本发明第七个目的是能使旧的，但可靠的车辆所有者用简易和有效的方法以维持调节顺从性。
本发明第八个目的是提供一种维持或再生催化柴油机颗粒物收集器的活性的方法。
这些和其他目的都可由本发明完成，从而提供了一种柴油机能在低颗粒物排放下运行的改进方法。
本发明方法包括：柴油机装上铂催化的颗粒物收集器，并以有效降低收集器的平衡点的量使用柴油机燃料和燃料可溶性铈组合物的混合物而使柴油机运行。优选的是，燃料还要含有燃料可溶的有机-铂族金属化合物，例如含有选自铂、钯、铑和这些金属中两种或更多种混合物的铂族金属。在另一实施方案中，有效的铂族金属化合物可在收集器前加入到废气中或燃料的空气中。
附图说明
借助于附图并阅读下列详细的描述，将会更好地理解本发明并且其优点将更为显而易见，其中：
图1是具有排气系统的柴油机示意图，其中所述系统包括按本发明的催化的颗粒物收集器；
图2是根据本发明使用的部分颗粒物收集器的放大、剖面示意图。
优选实施方案的详细描述
术语“柴油机”是指包括所有的压缩点火的引擎，用于动态的(包括船舶)和固定的动力装置并且是每次循环两冲程，每次循环四冲程以及旋转型的。
术语“烃燃料”是指包括所有由“馏出的燃料”或“石油”制备的那些燃料。术语“馏出的燃料”是指所有通过石油或石油馏份和残渣的蒸馏所制备的那些产物。术语“石油”就其通常含义意指包括所有那些不管其来源通常包括在术语含义中的物料，包括烃的物料，不管其粘度，它们是从矿物燃料中回收的。
术语“柴油机燃料”含义是“馏出的燃料”，包括满足ASTM对柴油机燃料所定义的柴油机燃料或其它燃料，即使它们不全是由馏份组成的而且还能包括醇、醚、有机硝基化合物和诸如此类(例如甲醇、乙醇、二乙醚、甲基乙基醚、硝基甲烷)。还有在本发明范围内的是由植物或矿物源如玉米、苜蓿、页岩和煤所产生的乳状液和液体燃料。这些燃料也可以含有本领域一般技术人员已知的其他添加剂，包括染料、十六烷改进剂、抗氧剂如2.6-二-叔-丁基-4-甲基酚、防腐蚀剂、防锈剂如烷基化的琥拍酸和酸酐、抑菌剂、防胶凝剂、金属失活剂、上部汽缸润滑剂。防冻剂等。
参考图1，它表示由箱11加入燃料的柴油机10。该燃料用适当的铈化合物并优选也用铂化合物进行催化。
在具体的铈化合物中有：乙酰基丙酮化铈(III)和各种铈皂如铈(III)的萘烷酸盐(napthanate)、辛酸铈、硬脂酸铈、新癸酸铈等。许多铈化合物都是满足化学式：Ce(OOCR)3的三价化合物，其中R＝烃，优选C2-C22，并且包括脂族、脂环族、芳基和烷芳基。化合物配合量在每百万份燃料约1-100ppm的铈(mg/l)，优选范围约5-30ppm。这含量能通过使用铈结合铂催化的颗粒物收集器的量而能明显低于目前所使用的。
从柴油机出来的废气将流过排气管12，它载带有来自燃料添加的铈催化剂组合物释放的催化金属，并且优选还含铂，进入催化颗粒物收集器14。收集器既可以按装配形式催化也可以通过引擎在有铂金属燃料添加剂存在下运行而造成催化剂沉积物而进行催化。收集器14可以是合适的耐热材料制的常规结构。所述材料例如是二氧化硅-氧化铝组合物，如堇青石、碳化硅、玻璃或金属纤维，多孔玻璃或金属基质，或诸如此类。铂催化的收集器是可市购并且根据文献报道在降低平衡点上是有效的。除了使用铂本身外，其他铂族金属也可以使用，例如组合起来使用。这种类型的收集器是在本发明规划中的(还可以是那些通过用其它方式如来自燃料添加剂以沉积铂族金属而催化的形式)且能降低平衡点的程度大于单独用铈添加剂催化的收集器或未催化的收集器。这样，使用有催化收集器的铈能使平衡点随铈含量的降低而降低。
参考图2，该图示意地表示放大的收集器截面，说明工艺过程的动力学。通道18其总数的约一半是沿着废气流的方向延伸(见箭头)，而总数的另一半通道沿相反方向延伸。通道沿废气流方向一端是封闭的，具有侧孔通向邻近的通道。通道的精确构型依据许多设计和制造的变化而不同，但重要的共同因素是颗粒物(例如图2中的小圆点20)因横移而被停止并且排出收集器。如果收集器继续有效时，这些颗粒物在收集器中必定被桡尽。因此，根据本发明，按特定方式使用具体催化物质以保证持续的低平衡点，例如在从约275到约400℃范围内，优选低于325℃。
再次参考图2，用铂催化收集器(铂以正方形22表示)。活性铈(在图2中以空心圆圈24表示)，是在燃料燃料时释放的，它由废气载带沉积在通道18中。铈在铂催化的收集器上的综合效应是以不可预测的方式明显降低平衡点。
如上所述，燃料优选地还含有燃料可溶性有机铂族金属化合物，例如，铂、钯或铑的一种。其中铂族金属化合物选自乙酰基丙酮化铂和具有通式XPtR1R2的化合物，式中X是含至少一种有烯、炔或芳族pi键构型的不饱和碳-碳键的配位体而且R1和R2分别是苄基、苯基、硝基苄基或1-10个碳原子的烷基，例如二苯基环辛二烯铂(11)。
适合的铂族金属化合物公开于例如在先的Bowers和Sprague的US专利4,892,562和4,891,050、Epperly和Sprague的5,034,020、Epperly、Sprague、Kelso和Bowers的5,215,652和Peter-Hoblyn，Epperly，Kelso和Sprague的5,266,083，Epperly、Sprague、Kelso和Bowers的WO 90/07561以及US专利申请号08/597,517，由Peter-Hoblyn，Valentine和Sprague于1996年1月31日申请，引入本文作为参考。该申请认为，这些化合物的混合物可以和一种或多种其他铂族金属化合物如皂、乙酰基丙酮化物、醇盐、β-二酮盐(β-diketonates)和磺酸盐例如将在下面更详细地描述的类型一起使用。
铂族金属催化剂和/或其他催化剂可以以对其预定目的有效的任何方式加入，如通过将其加到散装储存的燃料中，加到与柴油机连接的箱体中的燃料中，或通过连续或间歇加入，如通过合适的计量装置，例如图1中由罐32的30，而加入通向柴油机的燃料管线，或以蒸气、气体或气溶胶形式进入进气管，收集器前的废气，收集器后的废气但都在循环进入柴油机之前、或混合槽或等效的装置，其中废气与进来的空气混合。
当使用时，铂族金属催化剂组合物优选的使用量，按体积计每百万份燃料中有低于1份(按重量计)钯族金属(ppm)。当用于催化未催化的收集器(或已成失活的收集器)时，可以使用更高的配合量，例如从1到25(或更多)ppm，以实施催化剂在收集器中的快速沉积，对于本说明书来说，所有“每百万份”数字都基于重量/体积，即克/1×106cm3(也可以毫克/升表示)，并且百分比是按重量计，除非另有指示。助催化剂是以其预定目的有效含量使用，优选含量为所用燃料的1-200ppm，例如5-60ppm。
上面的描述是为了指导本领域一般技术人员如何实施本发明，而不是用来详述本发明所有明显的修改方案和变更方案，这些方案对熟练技术人员来说基于阅读本说明书是明显的，但可预料这些显而易见的修改方案和变更方案都包括在本发明的范围内，本发明是由下列权利要求书限定，权利要求书覆盖了满足本发明目的有效的所有装置和顺序中所指出的组成部分和步骤，除非上下文另有相反指示。

Claims (3)

1.一种使柴油机在低颗粒物排放下运行的方法，包括：
使柴油机装有铂催化颗粒物收集器，在废气通过其中时，收集器有效收集颗粒物，在使用前收集器用铂催化，以使收集器的平衡点在初始水平，并且
通过燃烧含有燃料可溶性铂族金属添加剂的柴油机燃料和燃料可溶性铈组合物的混合物而运行柴油机，以释放活性铈化合物进入废气，该废气将它们带入所述收集器，铈组合物的存在量使收集器的平衡点由其初始水平有效降低到持续低的水平。
2.按权利要求1所述的方法，其中，收集器含有二氧化硅-氧化铝的基质。
3.按权利要求2所述的方法，其中，收集器基质是堇青石。
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