CN112771256B - 三元催化剂 - Google Patents
三元催化剂 Download PDFInfo
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- CN112771256B CN112771256B CN201980057358.9A CN201980057358A CN112771256B CN 112771256 B CN112771256 B CN 112771256B CN 201980057358 A CN201980057358 A CN 201980057358A CN 112771256 B CN112771256 B CN 112771256B
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- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
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Abstract
本发明涉及一种催化剂,该催化剂包括在基材端部a和b之间延伸的长度(L)的载体基材以及三个洗涂层区A、B和C,其中洗涂层区A包含一种或多种第一铂族金属并且从基材端部a开始在长度(L)的一部分上延伸,洗涂层区C包含一种或多种第一铂族金属并且从基材端部b开始在长度(L)的一部分上延伸,并且洗涂层区B包含与洗涂层区A相同的组分以及另外的一种或多种第二铂族金属并且在洗涂层区A和C之间延伸,其中L=LA+LB+LC,其中LA是洗涂层区A的长度,LB是基材长度B的长度,并且LC是基材长度C的长度。
Description
技术领域
本发明涉及一种用于处理以主要化学计量的空气/燃料比运行的燃烧式发动机的废气的三元催化剂(TWC)。
背景技术
在燃烧式发动机领域中众所周知,燃料燃烧是不完全的,并且因此会产生污染物排放,如未燃烧的碳氢化合物(HC)、一氧化碳(CO)、氮氧化物(NOx)和颗粒物(PM)。为了改善空气质量,制定了排放限制法规,以实现来自固定应用和移动源的污染物低排放。对于客车之类的移动源,已经实施了主动策略诸如改善燃烧和优化A/F或λ控制,以努力减少污染物的排放。改善燃料-空气混合(A/F比)作为主要措施大幅减少了污染物。然而,由于这些年以来推行更为严格的法规,使用非均相催化剂已变得在所难免。
对于汽油发动机,所谓的三元催化剂(TWC)能够消除HC、CO和NOx。此类催化剂含有由一种或多种铂族金属(特别是铂、钯和/或铑)组成的催化活性材料。
TWC催化剂对CO、HC和NOx的最大转化率为约λ=1+/-0.005,其中空气/燃料比等于约14.56。高于这些值时,废气被称为稀薄的并含有过量的氧化剂诸如O2和NOx,并且CO和HC被催化氧化成二氧化碳和水。低于该值时,废气被称为富集的并含有过量的还原剂诸如H2、CO和HC,并且使用例如CO作为还原剂主要将NOx还原成氮气。
虽然在λ=1下实现了HC、CO和NOx的最大转化率,但汽油发动机在略微稀燃条件和略微富燃条件之间的连续振荡条件下运行。为了拓宽TWC的最佳运行,将铈-锆混合氧化物形式的储氧组分(OSC)包含在其配方中。
高度浓缩的铂族金属(PGM)如铂、钯和铑可在许多废气处理后应用中提供显著的性能改善。因此,就钯而言,通过在中等至严重老化之后将Pd载量从20g/ft3(0.7g/1)增加到100g/ft3(3.5g/l)的更高载量,起燃性能可改善100℃(测量为50%转化率的温度)。性能确实改善成高于这些载量,但是相对于钯载量的性能梯度是低的,并且需要非常高的钯载量以获得显著的影响。预计铑在TWC应用中有相同的一般趋势。
然而,三元转化催化剂中的高浓度铂族金属由于其高成本而并非首选。该缺点可通过策略性放置成靠近发动机歧管定位且具有高单元密度的小尺寸单块来部分地克服。该策略利用更热的废气温度,这缩短了冷启动的时间,因为单块加热更快。较低的质量与高单元密度相结合利用了较低的热惯性与更快热传递到紧密偶联(CC)单块相结合的优势。
用于改善起燃和用于降低铂族金属成本的另一个策略是将其选择性地定位在单块的一小部分上,通常小于单块体积的10%,在该体积中其具有最大益处。这允许我们在不使用大量铂族金属的同时浓缩铂族金属。
在文献中已知的是,当被施加到基材入口时,高度浓缩和短区的铂族金属由于改善的起燃而提供改善的冷启动性能,尤其是对于碳氢化合物(HC)氧化而言,因为当发动机冷却并且燃烧不完全时,高浓度的HC被排出。然而,紧密偶联单块可能在车辆的寿命期间暴露于保持在适当位置的多种污染物。这些包括来自发动机油的部分燃烧组分的分解,并且包括钙、磷、锌和硼。这些毒物不是均匀地沉积在单块的长度上,而是优先地朝向催化剂的入口沉积,并且随着朝向单块出口行进,它们的浓度快速下降。浓度的下降实际上可为指数级的,使得单块的前一英寸至两英寸可能具有非常高载量的这些组分。根据毒物进入废气的方式,观察到两种不同类型的中毒模式。如果毒物泄漏到车辆燃烧室中,则所得的磷和锌会渗入位于单块上的洗涂层(washcoat)并且与其组分(诸如铈和铝)反应。据信,磷在这种中毒机制中形成磷酸,并且其反应程度使得通常结构稳定的Ce-Zr混合氧化物分解得到新化合物。在极端情况下,铈可从Ce-Zr混合氧化物中提取以得到CePO4,这导致OSC性能损失。
在第二机制中,发动机油在其离开燃烧气缸之后可能直接泄漏到废气中。在这种情况下,将油直接沉积到单块洗涂层上并且分解以在表面上产生焦磷酸锌。如果经由该机制沉积高水平,则会在洗涂层表面上形成表面“釉面”或不可渗透屏障,使得废气分子无法扩散到洗涂层内的活性铂族金属组分。这通常被称为掩蔽,并且常见于严重油中毒的TWC催化剂。这种类型中毒的结果是,铂族金属带或区在单块的入口面处的选择性放置将适得其反,因为昂贵铂族金属中的很大一部分无法用于催化。
如果入口面受到源自歧管区的颗粒物诸如铁锈的冲击,则选择性地针对单块的入口区的其他中毒机制包括洗涂层侵蚀以及洗涂层的物理阻塞和涂覆。在世界上的一些国家诸如中国,辛烷值促进剂甲基-环-戊二烯基三羰基锰(MMT)的内含物可能在入口单块区上分解,以获得Mn3O4层,该Mn3O4层同样可用作必须渗透到洗涂层以发生催化的废气的物理掩蔽剂或阻断剂。
本发明的发明人讨论了是否可以通过将高铂族金属区定位在离单块的入口区足够远或足够靠后的位置来克服将具有高铂族金属浓度的单块的入口区分区(也被称为分带)的以上缺点,使得以上中毒和钝化机制最小化,同时仍然实现车辆上的改善起燃和随后更短的冷启动周期的优点。
在许多应用中,紧密偶联单块可能较长,高达4英寸至6英寸长。在这些类型的应用中,发明人出乎意料地发现,钯区可有利地且选择性地位于距入口面后部一英寸至四英寸处,以便受益于高钯浓度区的以下优点:改善起燃,同时避免钯区被油的分解产物、锈蚀或其他污染物诸如MMT衍生的沉积物覆盖或钝化的缺点。相比于对入口进行分区或在单块的整个体积上使用均匀的铂族金属分布,这种设计导致可测量的性能优势。本说明的部分可源自如上文所述的入口的选择性中毒外加当前CC-1单块的特殊特性(较小体积、较短部件、较低质量和较高单元密度)。
发明内容
本发明涉及一种催化剂,该催化剂包括在基材端部a和b之间延伸的长度L的载体基材以及三个洗涂层区A、B和C,其中
洗涂层区A包含一种或多种第一铂族金属并且从基材端部a开始在长度L的一部分上延伸,
洗涂层区C包含一种或多种第一铂族金属并且从基材端部b开始在长度L的一部分上延伸,并且
洗涂层区B包含与洗涂层区A相同的组分以及另外的一种或多种第二铂族金属并且在洗涂层区A和C之间延伸,其中L=LA+LB+LC,其中LA是洗涂层区A的长度,LB是洗涂层区B的长度,并且LC是洗涂层区C的长度。
因此,洗涂层区A从基材端部a开始在长度L的一部分上延伸,洗涂层区B跟随洗涂层区A并且在长度L的一部分上延伸,并且洗涂层区C跟随洗涂层区B并且延伸直至基材端部b,同时不存在或基本上不存在洗涂层区的重叠。
具体地讲,洗涂层区B包含与洗涂层区A相同的组分并且采用与洗涂层区A相同的量。
在本发明的一个优选实施方案中,洗涂层区A和C是相同的并且包含相同量的相同组分。在这种情况下,一种或多种第一铂族金属均匀地分布在载体基材的整个长度L上,而一种或多种第二铂族金属仅存在于洗涂层区B中。这进一步意味着洗涂层区B中铂族金属的总量分别高于洗涂层区A和C中铂族金属的总量。
第一铂族金属和第二铂族金属可以相同或可以不同,但彼此独立。例如,第一铂族金属为铂、钯和/或铑,并且第二铂族金属为铂、钯和/或铑。优选地,第一铂族金属为钯和铑,并且第二铂族金属为钯,或者第一铂族金属为钯和铑,并且第二铂族金属为铑。在另一个实施方案中,第一铂族金属为钯和铑,并且第二铂族金属为铂。
第二铂族金属也可以是铂和钯、铂和铑或钯和铑。
在第一铂族金属和第二铂族金属均相同(例如钯)的情况下,洗涂层区B包含比洗涂层区A和C更高量的铂族金属(例如钯)。
在本发明的一个实施方案中,
·洗涂层区A包括均在长度LA上延伸的两个洗涂层区A1和A2,其中洗涂层区A1包含一种或多种第一铂族金属,并且洗涂层区A2包含不同于洗涂层区A1的一种或多种第一铂族金属的一种或多种第一铂族金属,
·洗涂层区C包括均在长度LC上延伸的两个洗涂层区C1和C2,其中洗涂层区C1包含一种或多种第一铂族金属,并且洗涂层区C2包含不同于洗涂层区C1的一种或多种第一铂族金属的一种或多种第一铂族金属,并且
·洗涂层区B包括均在长度LB上延伸的两个洗涂层区B1和B2,其中洗涂层区B1包含与洗涂层区A1相同的组分,并且洗涂层区B2包含与洗涂层区A2相同的组分,并且其中洗涂层区B1和B2包含另外的一种或多种第二铂族金属。
在本发明的实施方案中,洗涂层区A2覆盖洗涂层区A1,洗涂层区B2覆盖洗涂层区B1,并且/或者洗涂层区C2覆盖洗涂层区C1。
在本发明的实施方案中,洗涂层区Al包含钯或包含钯以及一种或多种另外的铂族金属,具体地为铂和铑,优选地为铑,并且洗涂层区A2包含铑或包含铑以及一种或多种另外的铂族金属,具体地为铂和钯,优选地为钯。
优选地,洗涂层区A1中的第一铂族金属为钯,并且洗涂层区A2中的第一铂族金属为铑。在这种情况下,重量比Pd∶Rh为例如10∶1至1∶10。
类似地,洗涂层区C1包含钯或包含钯以及一种或多种另外的铂族金属,具体地为铂和铑,优选地为铑,并且洗涂层区C2包含铑或包含铑以及一种或多种另外的铂族金属,具体地为铂和钯,优选地为钯。
优选地,洗涂层区C1中的第一铂族金属为钯,并且洗涂层区C2中的第一铂族金属为铑。在这种情况下,重量比Pd∶Rh为例如10∶1至1∶10。
优选的是,洗涂层区A1和C1以及洗涂层区A2和C2分别是相同的并且包含相同量的相同组分。
在本发明的优选实施方案中,除了洗涂层区B中存在第二铂族金属之外,洗涂层区A、B和C是相同的并且包含相同量的相同组分。
同样,除了洗涂层区B1中存在第二铂族金属之外,洗涂层区A1、B1和C1是相同的,并且除了洗涂层区B2中存在第二铂族金属之外,洗涂层区A2、B2和C2是相同的并且包含相同量的相同组分。
如果在洗涂层区A和A1中的铂族金属分别包含钯并且在洗涂层区C和C1中的铂族金属分别包含钯的情况下,基于载体基材的区体积并以钯金属计算,其通常以0.04g/l至4.0g/l的量存在。
基于载体基材的体积并以钯金属计算,洗涂层区B和B1中的钯含量在这种情况下分别通常为2g/l至30g/l。
在洗涂层区A和A1中的铂族金属分别包含铑的情况下,基于载体基材的区体积并且并以铑金属计算,其通常以0.04g/l至4.0g/l的量存在。这同样分别适用于洗涂层区C和C1。
优选地,第一铂族金属和第二铂族金属彼此独立地承载在载体材料上。
作为载体材料,可以使用本领域技术人员已知的所有材料。通常,它们的BET表面积为30m2/g至250m2/g,优选地为100m2/g至200m2/g(根据德国标准DIN 66132确定),并且具体地选自由以下项组成的组:氧化铝、二氧化硅、氧化镁、二氧化钛、氧化锆、二氧化铈、包含这些材料中的至少一种的混合物以及包含这些材料中的至少一种的混合氧化物。
优选氧化铝、氧化铝/二氧化硅混合氧化物、氧化镁/氧化铝混合氧化物、二氧化铈、二氧化铈/氧化锆混合氧化物和沸石。
在使用氧化铝的情况下,优选例如用1重量%至10重量%、特别是1重量%至4重量%的氧化镧使其稳定。
不同的铂族金属可承载在相同或不同的载体材料上。
在本发明的实施方案中,洗涂层区A在载体基材的长度L的15%至50%、优选地20%至40%上延伸,洗涂层区B在载体基材的长度L的7%至30%、优选地15%至25%上延伸,并且洗涂层区C在载体基材的长度L的20%至78%、优选地35%至65%上延伸。
在本发明的实施方案中,长度L的载体基材可为流通式基材或过滤基材。此类载体基材通常由堇青石、金属或纤维材料制成,并且在文献中有描述,并且可在市场上购得。
本发明的其中洗涂层区A和C是相同的催化剂可由已知方法特别是由四步法制造,该方法包括
·用涂层悬浮液(洗涂层)涂覆载体基材,该涂层悬浮液在载体基材的整个长度L上含有洗涂层区A的组分,
·在长度LA上施加从基材端部a延伸的疏水掩蔽区,
·将涂覆的载体基材浸渍在含有第二铂族金属的水溶性化合物的水性溶液中,从基材端部a开始,直到长度LA+LB,以便形成洗涂层区B,以及
·干燥并加热涂覆的载体基材以便去除掩蔽区。
第一步骤中的涂覆通常经由常规的浸渍、抽吸和泵送方法进行,这些方法在文献中被广泛描述并且是本领域的技术人员已知的。
在第二步骤中,可使用多种方法来施加疏水掩蔽区。
在一种方法中,可使用熔点恰好高于室温的蜡或粘性油,并且该蜡或粘性油在熔融时具有低粘度,从而允许我们使用活塞式涂布机将熔融的蜡推入单块中并且通过活塞回缩去除过量的蜡或粘性油,以便在洗涂层表面上提供具有蜡或粘性油的残余层的清除通道。区长度可由活塞行程的长度精确地控制。可使用多种蜡类型,诸如可衍生自石油、煤炭或油页岩的石蜡。其它类型的蜡或粘性油可由乙烯聚合或丙烯聚合来合成。蜡或粘性油通常由一系列碳数在20至70个碳原子范围内的烃组成,其中以烷烃组分为主。然而,它们还可含有一系列官能团,诸如脂肪酸、伯长链醇和仲长链醇、不饱和键、芳族化合物、酰胺、酮和脂肪酸酯。
蜡的熔融温度既可通过链中的碳数或通过支链化的控制来控制,又可通过上述官能团的存在来控制。通常,需要恰好高于室温时熔融的蜡,诸如在约37℃(99°F)下熔融并且具有高于370℃的沸点的石蜡。其它蜡或油包括源自天然的产品,诸如椰子油、可可脂或具有适当粘度和熔融温度的其它产品。
另选的方法是使用具有高固体含量的蜡乳液。该方法不需要加热蜡或油来获得适当粘度和流动性。在施加乳液之后,可将部件加热短时间以将蜡熔融并铺展在洗涂层表面上,从而在洗涂层上形成连续疏水层。
可用于本发明方法中的蜡和蜡乳液是技术人员已知的,并且可在市场上购得。
在第三步骤中使用的第二铂族金属的水溶性化合物可为任何稳定的铂族金属盐,包括硝酸盐、乙酸盐、氯化物、亚硫酸盐、胺络合物等。优选的是,溶液为中性或接近中性的并且无腐蚀性,诸如乙酸盐,如四胺乙酸钯。由于在基材通道中铂族金属溶液与洗涂层接触之后发生溶剂诸如水的芯吸,因此通常需要添加表面活性剂或表面张力调节剂以控制该现象,因为在没有表面活性剂或表面张力调节剂的情况下不能控制带长。
施加洗涂层区B的优选方法是使用精密活塞式涂布机,其中疏水掩蔽区和待与铂族金属溶液接触的区的确切长度是已知的。由于高浓度洗涂层区B的施加是在施加洗涂层之后完成的,因此该方法非常灵活,并且在洗涂层组合物或洗涂层通过次数方面不是技术专有的。
第二铂族金属的溶液横穿掩蔽区但铂族金属未被吸附,而吸附仅发生在洗涂层的超过掩蔽区的区上。通过了解掩蔽区的长度,可容易地确定和控制该区的长度。
第四步骤包括干燥涂覆的基材并将其加热至疏水掩蔽区被完全烧尽的温度。这些温度通常介于400℃和600℃之间。
第一步骤至第四步骤之后通常是煅烧和任选地在含有形成气体的气氛中进行热还原。
本发明的催化剂适用于处理以主要化学计量的空气/燃料比运行的燃烧式发动机的废气,该废气的处理通过使废气经过本发明的催化剂来实施。具体地讲,本发明的催化剂可以有利地用于紧密偶联的位置,优选地用作直接位于排气歧管后面(所谓的CC-1位置)的第一催化剂。
因此,本发明还涉及一种用于处理以主要化学计量的空气/燃料比运行的发动机的废气的方法,其特征在于废气经过本发明的催化剂,其中废气在基材端部a处进入催化剂并且在基材端部b处离开催化剂。
在该方法的一个优选实施方案中,本发明的催化剂被布置在紧密偶联的位置,特别是直接布置在排气歧管后面。
本发明的催化剂可与另一种三元催化剂、汽油颗粒过滤器、HC捕集器和/或NOx捕集器结合以形成三元催化剂体系。
例如,本发明的催化剂的基材端部b之后可以是常规的三元催化剂。
另外,本发明的催化剂的基材端部b可跟随常规的三元催化剂。
作为常规的三元催化剂,可使用本领域技术人员已知的且文献中所述的所有三元催化剂。通常,它们包含承载在载体材料上的铂族金属,特别是钯和铑,以及特别是铈-锆混合氧化物的储氧组分(OSC)。
除了使用本发明的催化剂来处理以主要化学计量的空气/燃料比运行的发动机的废气之外,其还可用作柴油机氧化催化剂来处理从稀燃发动机如柴油发动机排放的废气。
因此,本发明还涉及一种用于处理稀燃发动机的废气的方法,其特征在于废气经过本发明的催化剂,其中废气在基材端部a处进入催化剂并且在基材端部b处离开催化剂。
当用作柴油机氧化催化剂时,本发明的催化剂可与用于处理稀燃废气的催化剂体系的其它组分组合。此类组分的示例为主动NOx储存催化剂、被动NOx储存催化剂、柴油颗粒过滤器和SCR催化剂。
附图说明
图1示出了根据本发明的催化剂。附图的上部示出了本发明的催化剂(1)的细节,该催化剂包含载体基材(3),该载体基材在基材端部a和b之间延伸并且承载洗涂层区A(4)、洗涂层区B(5)和洗涂层区C(6)。
附图的下部示出了本发明的另一个实施方案的细节。催化剂(2)包含在基材端部a和b之间延伸的载体基材(3)。洗涂层区A包括洗涂层区A1(7)和A2(8),洗涂层区B包括洗涂层区B1(9)和洗涂层区B2(10),而洗涂层区C包括洗涂层区C1(11)和洗涂层区C2(12)。洗涂层区A1(7)和B1(9)的不同之处仅在于B1(9)包含与A1(7)相比的第二铂族金属。同样,洗涂层区A2(8)和B2(10)的不同之处仅在于B2(10)包含与A2(8)相比的第二铂族金属。
图2示出了根据本发明的催化剂体系。
上部示出了本发明的催化剂体系(13),该催化剂体系包含本发明的催化剂(1)和常规的三元催化剂(15)。两种催化剂被布置成使得洗涂层区C(6)之后是常规的三元催化剂(15)。
下部示出了本发明的催化剂体系(14),该催化剂体系包含本发明的催化剂(1)和常规的三元催化剂(15)。两种催化剂被布置成使得洗涂层区C(6)跟随常规的三元催化剂(10)。
图3示出了根据纵向剖开的实施例1的催化剂C1的照片。显然,洗涂层区A、B和C已按预期施加。
图4示出了根据实施例1的催化剂C1的洗涂层区A、B和C在施加掩蔽剂和Pd溶液浸渍之后的Pd载量。
图5示出了根据纵向剖开的实施例2的催化剂C2的照片。显然,洗涂层区A、B和C已按预期施加。
图6示出了根据实施例2的催化剂C2的洗涂层区A、B和C在施加掩蔽剂和Pd溶液浸渍之后的Pd载量。
具体实施方式
比较例1
比较例1是1层Pd/Rh技术,其制备如下:
称量所需量的水,并以待制备浆液的最终固体含量的0.5重量%添加HNO3。然后添加含有3重量%La2O3的稳定氧化铝以进行稳定,之后添加等量的含有4重量%La2O3的第二高孔隙率稳定氧化铝。然后在搅拌下添加BaSO4,之后添加乙酸镧,并且最后添加OSC物质。OSC物质由CeO2=40重量%、ZrO2+HfO2=50重量%、La2O3=5.0重量%和Pr6O11=5.0重量%组成。然后使用Sweco型研磨机将浆液研磨至5微米至7微米的平均粒度,90%的直径分布为18微米至20微米,并且100%通过小于45微米(即,100%的颗粒具有小于45微米的粒度)。然后称量浆液,并且在540℃下测量LOI(烧失量)以确定总煅烧固体含量。基于该值,计算Pd和Rh量以得出基于2.85g/in3或174g/L的最终煅烧洗涂层载量的目标载量。首先滴加硝酸铑,之后搅拌15分钟,并且然后在搅拌下以硝酸钯的形式滴加Pd。在添加Pd之后,根据洗涂层载量目标和待涂覆的基材类型,将浆液比重调节至1.4至1.6的范围。
将蜂窝陶瓷单块(可商购获得的流通式基材,由堇青石制成,3.66英寸圆×6.0英寸长,400cpsi,6.5铣削壁厚)的一个端部浸渍到洗涂层浆液中,之后使用真空将浆液抽吸到通道中,以此执行涂覆。然后从浆液中移除单块,并且通过向其另一端部施加真空来清除通道。通过改变比重和其他涂层参数(诸如真空时间和抽吸到蜂窝通道中的浆液的量)来控制洗涂层载量。在施加洗涂层之后,将单块在540℃下煅烧2小时。基于干燥煅烧,最终WC载量为稳定的氧化铝=80g/L、BaSO4=13g/L、OSC=80g/L和La2O3=1.6g/L,得到总载量174g/L。在单块的总长度上涂覆洗涂层。两个样品以不同的PGM载量构建,一个以Pd载量为50g/ft3和Rh=3.0g/ft3(CC1)构建,并且第二个以Pd=14g/ft3和Rh=1.0g/ft3(CC2)构建。
实施例1(C1)
本发明的PGM分带或分区催化剂如下制备。在本实施例中,使用比较例1的高Pd载量的单块CC1,其中WC载量为174g/L并且Pd载量为50g/ft3。通过将单块的一个端部浸渍在纯可可脂中来施加掩蔽带,该纯可可脂在水浴中被加热至50℃以提供可容易地流入单块通道中并被注入至16mm的长度的低粘度流体。可可脂在38℃的温度下熔融。通过将强制风从单块的相对端吹过单块通道来去除通道中的过量掩蔽剂。使分带部件在室温下的空气中静置12小时,使得掩蔽剂冷却至室温,并且在部件入口处的洗涂层上形成实心均匀的不透水层。
Pd带或区的施加如下进行。制备由增稠剂在水中组成的水性溶液,其中所用的增稠剂是商业多糖。当施加水性Pd溶液以获得分带区时,添加增稠剂以控制和限制水性Pd溶液的芯吸。基于溶液的总重量,增稠剂以0.5重量%添加。还可使用不同的表面活性剂来降低Pd溶液的表面张力并且最小化芯吸,从而改善对Pd带长的控制。向该溶液中添加四胺乙酸钯,其浓度基于分带区中的Pd载量目标、带/区长度以及在无溶液或Pd摄取的情况下注入到掩蔽区上时达到分带区的端部所需的溶液量来确定。为了测定Pd溶液浓度,使用不存在Pd盐的多糖在水中的溶液来测量单块的初始湿重摄取。在本实施例中,掩蔽区长度为16mm并且目标Pd区/带长度为49mm。计算的溶液摄取的重量为73.5克,其中Pd浓度为28.5mg/g溶液。在施加Pd带之后,通过真空从单块的注入端去除过量的溶液。然后将分带/分区部件在上流式鼓风烘箱中煅烧,其中掩蔽带位于单块的顶部处。煅烧温度为550℃,持续2小时。煅烧之后,将部件纵向剖开,以确认带/区已按预期施加。图3所示的照片确认带/区是按预期施加的。此外,从区A、B和C移除单块切片,并且使用ICP(电感耦合等离子体)分析来测量Pd含量,并且在图4中数据以每个区的g/ft3Pd表示。根据图4所示的Pd分析,显而易见的是,高Pd浓度带/区被成功地施加。
实施例2(C2)
在第二分带实验中,具有较低Pd载量(Pd=14g/ft3)的比较例1的单块CC2如实施例1所述进行分带。在这种情况下,目标Pd区长度为74mm,其中前掩蔽区长度为16mm,如实施例1所述。计算的溶液摄取量为112.9克,其中Pd浓度为28.5mg/g。煅烧之后,将部件纵向剖成两半,并且所得的带可视化示于图5中,证实已实现预期的分带。在图6中,示出了对取自区A、B和C的单块切片进行ICP分析之后的Pd载量的结果。显然,Pd带被成功地施加。
Claims (21)
1.三元催化剂,所述催化剂包括在基材端部a和b之间延伸的长度L的载体基材以及三个洗涂层区A、B和C,其中
洗涂层区A包含一种或多种第一铂族金属并且从基材端部a开始在所述长度L的一部分上延伸,
洗涂层区C包含一种或多种第一铂族金属并且从基材端部b开始在所述长度L的一部分上延伸,并且
洗涂层区B包含与洗涂层区A相同的组分以及另外的一种或多种第二铂族金属并且在洗涂层区A和C之间延伸,其中L=LA+LB+LC,其中LA是洗涂层区A的长度,LB是洗涂层区B的长度,并且LC是洗涂层区C的长度;
其中洗涂层区A和C是相同的并且包含相同量的相同组分;
所述一种或多种第一铂族金属均匀地分布在载体基材的整个长度L上,而所述一种或多种第二铂族金属仅存在于洗涂层区B中。
2.根据权利要求1所述的三元催化剂,其中第一铂族金属和第二铂族金属是相同的或不同的。
3.根据权利要求1或2所述的三元催化剂,其中所述第一铂族金属为铂、钯和/或铑,并且所述第二铂族金属为铂、钯或铑。
4.根据权利要求1或2所述的三元催化剂,其中所述第一铂族金属为钯和铑,并且所述第二铂族金属为钯。
5.根据权利要求1或2所述的三元催化剂,其中所述第一铂族金属为钯和铑,并且所述第二铂族金属为铑。
6.根据权利要求1或2所述的三元催化剂,其中所述第一铂族金属为钯和铑,并且所述第二铂族金属为铂。
7.根据权利要求1或2所述的三元催化剂,其中
·洗涂层区A包括均在所述长度LA上延伸的两个洗涂层区A1和A2,其中洗涂层区A1包含一种或多种第一铂族金属,并且洗涂层区A2包含不同于洗涂层区A1的所述一种或多种第一铂族金属的一种或多种第一铂族金属,
·洗涂层区C包括均在所述长度LC上延伸的两个洗涂层区C1和C2,其中洗涂层区C1包含一种或多种第一铂族金属,并且洗涂层区C2包含不同于洗涂层区C1的所述一种或多种第一铂族金属的一种或多种第一铂族金属,并且
·洗涂层区B包括均在所述长度LB上延伸的两个洗涂层区B1和B2,其中洗涂层区B1包含与洗涂层区A1相同的组分,并且洗涂层区B2包含与洗涂层区A2相同的组分,并且其中洗涂层区B1和B2另外包含一种或多种第二铂族金属。
8.根据权利要求7所述的三元催化剂,其中洗涂层区A1中的所述第一铂族金属为钯和/或铑,并且洗涂层区A2中的所述第一铂族金属为铑。
9.根据权利要求7所述的三元催化剂,其中洗涂层区A1中的所述第一铂族金属为钯和铑,并且重量比Pd:Rh为10:1至1:10。
10.根据权利要求1或2所述的三元催化剂,其中所述第一铂族金属和所述第二铂族金属彼此独立地承载在载体材料上。
11.根据权利要求10所述的三元催化剂,其中所述载体材料选自由以下项组成的组:氧化铝、二氧化硅、氧化镁、二氧化钛、氧化锆、二氧化铈、包含这些材料中的至少一种的混合物以及包含这些材料中的至少一种的混合氧化物。
12.根据权利要求1或2所述的三元催化剂,其中洗涂层区A在所述载体基材的所述长度L的15%至50%上延伸,洗涂层区B在所述载体基材的所述长度L的7%至30%上延伸,并且洗涂层区C在所述载体基材的所述长度L的20%至78%上延伸。
13.根据权利要求1或2所述的三元催化剂,其中所述长度L的所述载体基材为流通式基材。
14.根据权利要求1或2所述的三元催化剂,其中所述长度L的所述载体基材为过滤基材。
15.制造根据权利要求1至14中的任一项所述的三元催化剂的方法,通过四步法进行,所述方法包括:
·采用用于形成洗涂层的涂层悬浮液涂覆所述载体基材,所述涂层悬浮液在所述载体基材的整个长度L上含有洗涂层区A的组分,
·在所述长度LA上施加从基材端部a延伸的疏水掩蔽区,
·将所述涂覆的载体基材浸渍在含有所述第二铂族金属的水溶性化合物的水性溶液中,从基材端部a开始,直到所述长度LA+LB,以便形成洗涂层区B,以及
·干燥并加热所述涂覆的载体基材以便去除所述掩蔽区。
16.催化剂体系,所述催化剂体系包含根据权利要求1至14中的任一项所述的三元催化剂以及另一种三元催化剂、汽油颗粒过滤器、HC捕集器和/或NOx捕集器。
17.根据权利要求16所述的催化剂体系,其中根据权利要求1至14中的任一项所述的三元催化剂的基材端部b之后是另一种三元催化剂。
18.根据权利要求16所述的催化剂体系,其中根据权利要求1至14中的任一项所述的三元催化剂的基材端部b跟随另一种三元催化剂。
19.用于处理燃烧式发动机的废气的方法,其中所述废气经过根据权利要求1至14中的任一项所述的三元催化剂,其中所述废气在基材端部a处进入所述催化剂并且在基材端部b处离开所述催化剂。
20.根据权利要求19所述的方法,其中根据权利要求1至14中的任一项所述的三元催化剂被布置在紧密偶联的位置。
21.用于处理稀燃发动机的废气的方法,其特征在于所述废气经过根据权利要求1至14中的任一项所述的三元催化剂,其中所述废气在基材端部a处进入所述催化剂并且在基材端部b处离开所述催化剂。
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