CN109152987A - 具有超低pgm载量的协同pgm作为内燃机的紧耦合三元催化剂的用途 - Google Patents
具有超低pgm载量的协同pgm作为内燃机的紧耦合三元催化剂的用途 Download PDFInfo
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Abstract
公开了具有不同材料组成和配置的用作紧耦合(CC)三元催化剂(TWC)系统的具有超低PGM载量的协同铂族金属(SPGM)。SPGM CC催化剂(其中二元或三元尖晶石结构的ZPGM组合物负载到载体氧化物上)与商品化PGM UF催化剂结合并在TGDI和PI发动机内根据Federal Test Procedure FTP‑75测试。将包括SPGM CC(具有超低PGM载量)催化剂和商品化PGM UF催化剂的TWC系统的性能与商品化PGM CC和PGM UF催化剂的性能比较。所公开的TWC系统表明,SPGM CC TWC催化性能相当于或甚至超过高PGM基传统TWC催化剂,具有降低的尾管排放。
Description
背景
公开领域
本公开大体上涉及三元催化剂(TWC)系统,更特别涉及用于减少来自发动机排气系统的排放的以紧耦合配置使用的具有超低PGM载量的协同PGM TWC催化剂。
背景信息
三元催化剂(TWC)系统继续作为车辆内燃机的主要排放控制策略实施。但是,汽车行业最近已开启一个快速发展与能量效率相关联的发动机/燃烧改进的生产路线图的时期。相关的催化剂改进需要超越对铂族金属(PGM)用量和用作储氧材料(OSM)的稀土(RE)金属的细调并为催化剂开发商带来重要的挑战。
从轻型和重型排放标准的全球收紧注意到的更严格尾气法规趋势在现代催化剂的开发中带来重要的改进,包括:改进的燃料经济性和温室气体排放减少、其建立较低排气温度的要求;和由于它们的可得性和价格波动而与PGM材料的供应和需求相关的材料供应问题。
由于催化剂配方的改变持续提高TWC系统的成本,对催化性能显著的催化剂的需要已将努力引向开发能够提供所需协同效应以实现更高催化性能的催化材料。另外,遵守更严格的环境法规和对更低制造成本的需求需要新型TWC系统。因此,仍然需要提供使用减少量的PGM催化剂材料并且不含RE金属、表现出与使用标准量的PGM催化剂材料和RE金属的传统TWC系统所表现的催化性质基本类似或更高的催化性质的TWC系统。
概述
本公开描述了包括协同超低铂族金属(PGM)载量紧耦合(CC)催化剂的三元催化剂(TWC)。TWC系统内的超低PGM载量CC催化剂与包含尖晶石氧化物材料的零PGM(ZPGM)催化剂材料组合物协同增效。SPGMCC催化剂的ZPGM层内的催化剂材料组合物包括负载到载体氧化物上的二元或三元尖晶石结构。PGM层内的催化剂材料组合物包括负载到载体氧化物上的具有在大约1g/ft3至大约10g/ft3的范围内的超低浓度的可变铂(Pt)/钯(Pd)/铑(Rh)。
在一些实施方案中,配置各种TWC系统以评估它们的催化性质,根据U.S.FederalTest Procedure(FTP-75)规程测量尾气排放。在这些实施方案中,配置TWC系统以包括市售地板下(UF)催化剂和SPGM(具有超低PGM)CC催化剂。由这些实施方案进一步地,将包括SPGMCC催化剂的配置TWC系统与内燃机,尤其例如Tier 2bin 4涡轮汽油直喷(TGDI)发动机或自然吸气式进气口喷射(port injection,PI)发动机机械耦合并流体连通,以进行根据FTP-75规程的排放认证测试。
在另一些实施方案中,用市售PGM基OEM CC和PGM基OEM和售后市场(aftermarket)UF催化剂配置标准TWC系统。在这些实施方案中,将该标准TWC系统与用于根据FTP-75规程测试包括超低载量SPGMCC催化剂的上述TWC系统的基本类似的发动机机械耦合并流体连通。
在进一步实施方案中,在根据FTP-75规程的排放测试之前,TWC系统内的OEM CC、OEM UF和SPGM CC催化剂在发动机台架上使用标准多模式老化循环(对于CC和UF催化剂分别在大约1000℃和大约900℃的床温度下大约50小时)老化。
在一些实施方案中,根据FTP-75规程评估对上述TWC系统在尾管下游测得的(加权袋结果)SPGM CC催化剂的催化效率并进一步与对CC高PGM OEM催化剂测得的加权排放比较。
在一个实施方案中,本公开涉及一种用于处理内燃机的排气料流的催化系统,其包含内燃机;配置成接收来自所述内燃机的至少一个排气料流的紧耦合催化转化器,其中所述紧耦合催化转化器包含含有尖晶石催化剂组合物和超低铂族金属催化剂材料的协同铂族金属催化剂,并且其中所述铂族金属催化剂材料具有大约1g/ft3至大约10g/ft3的铂族金属浓度;和在所述紧耦合催化转化器下游并与其流体连通的地板下催化转化器,其中所述地板下催化转化器包含铂族金属催化剂。
在一个实施方案中,所述地板下催化转化器具有大约10至100g/ft3,更通常大约15至60g/ft3的铂族金属浓度。
在一些实施方案中,所述地板下催化转化器的铂族金属选自铂、钯、钌、铱和铑。在一个优选实施方案中,所述地板下催化转化器的铂族金属包含铂和铑的组合。
所述协同铂族金属催化剂的尖晶石催化剂组合物可包含具有通式AxB3-xO4的二元尖晶石,其中X为0.01至2.99,且A和B选自钠、钾、钙、钡、锌、镉、铝、镁、锰、镍、铜、钴、铁、铬、钛、铈、锶、镧、镨、钕、钐、铟及其混合物。
例如,所述二元尖晶石可包含Ni-Fe尖晶石,例如含Ni0.5Fe2.5O4的Ni-Fe尖晶石结构。
在一些实施方案中,所述尖晶石催化剂组合物包含至少一种基底(substrate),和含有具有式AXBYM3-X-Y的尖晶石氧化物的催化剂组合物,其中X为大约0.01至大约1.99且Y为大约0.01至大约1.0,且其中A、B和M彼此不同并选自钠、钾、钙、钡、锌、镉、铝、镁、锰、镍、铜、钴、铁、铬、钛、铈、锶、镧、镨、钕、钐、铟及其混合物。
在一个实施方案中,所述尖晶石催化剂组合物负载到选自Al2O3、掺杂Al2O3、ZrO2、掺杂ZrO2、SiO2、掺杂SiO2、TiO2、掺杂TiO2、掺杂Al2O3-ZrO2、Nb2O5及其混合物的载体氧化物上。
在一个实施方案中,所述尖晶石催化剂组合物作为洗涂层沉积到基底上,且所述超低铂族金属催化剂材料作为外覆涂层沉积到所述洗涂层上。在其上沉积所述尖晶石催化剂组合物的合适基底的一个实例是陶瓷,如堇青石。
在一个实施方案中,所述超低铂族金属催化剂的铂族金属选自铂、钯、钌、铱和铑。在一个优选实施方案中,所述超低铂族金属催化剂的铂族金属包含铂和铑的组合。在一个特定实施方案中,所述超低铂族金属催化剂材料中的铂量为大约1至10g/ft3,且所述超低铂族金属催化剂材料中的铑量为大约1至10g/ft3。
在一个实施方案中,所述超低铂族金属催化剂材料包含铂和铑的组合。通常,铂和铑可以任何比率存在,如1:10至10:1。在一个优选实施方案中,所述超低铂族金属催化剂材料包含以1:1比率存在的铂和铑的组合。
在一个实施方案中,所述尖晶石催化剂组合物包含负载到掺杂Al2O3-ZrO2载体氧化物上的Ni-Fe二元尖晶石结构。
在一些实施方案中,所述地板下催化转化器包含铂和铑的组合,其中所述地板下催化转化器中的铂族金属总量为大约15至25g/ft3。
在一些实施方案中,所述协同铂族金属催化剂的铂族金属催化剂不含稀土金属和储氧材料。
有利地,所述催化系统的实施方案表现出与具有铂族金属催化剂代替协同铂族金属催化剂作为紧耦合催化转化器的类似系统相比NOx、CO和THC的尾管排放的降低。
在另一实施方案中,本公开提供一种从内燃机排气料流中除去污染物的方法。例如,所述方法可包括以下步骤:将内燃机排气料流引入包含含有尖晶石催化剂组合物和超低铂族金属催化剂材料的协同铂族金属催化剂的紧耦合催化转化器,其中所述铂族金属催化剂具有大约1g/ft3至大约10g/ft3的浓度由此至少部分催化转化NOx、CO和THC;和将所述至少部分催化转化的排气料流引入包含铂族金属催化剂的地板下催化转化器。
在一个优选实施方案中,所述尖晶石催化剂组合物包含负载到掺杂Al2O3-ZrO2载体氧化物上的Ni-Fe二元尖晶石结构。
从与附图一起作出的下列详述中可看出本公开的许多其它方面、特征和益处。
附图简述
参照下列附图可以更好地理解本公开。附图中的组件不必成比例,而是着重于图解本公开的原理。在附图中,标号是指不同视图中的相应部件。
图1是图解根据一个实施方案的包括紧耦合(CC)和地板下(UF)催化剂的三元催化剂(TWC)系统的配置的图示。
图2是图解根据一个实施方案的用于CC用途的协同PGM(SPGM)催化剂的催化剂配置的图示。
图3是图解根据一个实施方案用于SPGM CC催化剂的发动机台架老化的标准多模式老化循环规程的图示。
图4是图解根据一个实施方案用于测试、测量和诊断如图1和2中所述的TWC系统的催化性能的U.S.Federal Test Procedure(FTP-75)的行驶阶段(driving phases)的图示。
图5是图解根据一个实施方案使用如图4中所述的FTP-75试验规程的涡轮汽油直喷(TGDI)发动机内所用的TWC系统1和2(如上所述)的尾管处加权NOX(克/英里)值的图示。
图6是图解根据一个实施方案使用如图4中所述的FTP-75试验规程的TGDI发动机内所用的TWC系统1和2(如上所述)的尾管处加权CO(克/英里)值的图示。
图7是图解根据一个实施方案使用如图4中所述的FTP-75试验规程的TGDI发动机内所用的TWC系统1和2(如上所述)的尾管处加权THC(克/英里)值的图示。
图8是图解根据一个实施方案使用如图4中所述的FTP-75试验规程的TGDI发动机内所用的TWC系统1和2(如上所述)的尾管处加权非甲烷烃(NMHC)(克/英里)值的图示。
图9是图解根据一个实施方案TWC系统1和2(如上所述)和使用在给定速度下的TGDI发动机的累积中尾管NOX排放结果的图示。
图10是图解根据一个实施方案TWC系统1和2(如上所述)和使用在给定速度下的TGDI发动机的累积中尾管THC排放结果的图示。
图11是图解根据一个实施方案使用如图4中所述的FTP-75试验规程的自然吸气式进气口喷射(PI)发动机内所用的TWC系统3和4(如上所述)的尾管处加权NOX(克/英里)值的图示。
详述
在此参照构成本文的一部分的附图中所示的实施方案详细描述本公开。可以使用其它实施方案和/或可以作出其它修改而不背离本公开的范围或精神。详述中描述的示例性实施方案无意限制提出的主题。
定义
本文所用的下列术语具有下列定义:
“空气-燃料比(AFR)”是指在燃烧过程中,如在内燃机中存在的空气与燃料的质量比。
“煅烧”是指在空气存在下在低于固体材料的熔点的温度下施加于固体材料以引起热分解、相变或除去挥发分的热处理过程。
“催化剂”是指可用于一种或多种其它材料的转化的一种或多种材料。
“催化转化器”是指通过催化氧化还原反应(氧化、还原或两者)将排气中的有毒污染物转化成较低毒污染物的车辆排放控制装置。
“催化剂系统”是指由包含基底、洗涂层和/或外覆涂层的至少两个层的包括催化剂,如PGM催化剂或ZPGM催化剂的任何系统。
“紧耦合催化剂(CCC)”是指位置很靠近发动机的排气歧管的催化剂。
“转化”是指至少一种材料化学变化成一种或多种其它材料。
“U.S.Federal Test Procedure(FTP)排放试验”是指在美国轻型车辆的排放认证测试程序。
“浸渍”是指用液体化合物灌注或饱和固体层或一些元素经介质或物质扩散的过程。
“初湿(IW)”是指将催化材料的溶液添加到干载体氧化物粉末中直至载体氧化物的所有孔隙体积被溶液填满且混合物达到接近饱和点的过程。
“λ”是指实际空气-燃料比与化学计量空气-燃料比的比率。
“研磨”是指将固体材料粉碎成所需的颗粒或粒子大小的操作。
“原始设备制造商(OEM)是指新车制造商或原始安装在新车的认证排放控制系统中的任何部件或组件的制造商。
“外覆(OC)涂层”是指可沉积到至少一个洗涂层或浸渍层上的至少一个涂层的催化剂层。
“铂族金属(PGM)”是指铂、钯、钌、铱、锇和铑。
“尖晶石”是指通式AB2O4的任何矿物,其中A离子和B离子各自选自矿物氧化物,尤其例如镁、铁、锌、锰、铝、铬、钛、镍、钴或铜。
“基底”是指提供足以沉积洗涂层和/或外覆涂层的表面积的任何形状或配置的任何材料。
“载体氧化物”是指用于提供有助于氧分布和催化剂暴露在反应物,例如NOX、CO和烃下的高表面积的多孔固体氧化物,通常为混合金属氧化物。
“协同PGM(SPGM)催化剂”是指使用不同催化剂配置的用ZPGM化合物协同增效的PGM催化剂系统。
“三元催化剂(TWC)”是指同时执行氮氧化物还原成氮气和氧气、一氧化碳氧化成二氧化碳和未燃烃氧化成二氧化碳和水的三个任务的催化剂。
“地板下(UF)催化剂”是指并入机动车的排气系统中、通常位于车辆地板下方、机械耦合到紧耦合(CC)催化剂下游的催化剂。
“洗涂(WC)层”是指可沉积到基底上的包括至少一种氧化物固体的至少一个涂层的催化剂层。
“零PGM(ZPGM)催化剂”是指完全或基本不含铂族金属(PGM)的催化剂。
公开描述
本公开描述了以包括与尖晶石基ZPGM组合物协同的超低PGM组合物的催化剂配置制成的协同铂族金属(SPGM)紧耦合(CC)三元催化剂,其不含稀土(RE)金属组合物。这些SPGM CC催化剂作为TWC转化器的组分并入发动机系统内,TWC转化器是用于控制和减少发动机废气排放的TWC系统的一部分。使用U.S.Federal Test Procedure(FTP-75)规程(2014)中描述的行驶阶段评估和比较这些TWC系统的转化性能。
TWC系统配置
图1是图解根据一个实施方案的包括紧耦合(CC)和地板下(UF)催化剂的三元催化剂(TWC)系统的配置的图示。在图1中,发动机系统100包括发动机102和TWC系统104。TWC系统104进一步包括紧耦合(CC)催化剂106和地板下(UF)催化剂108。在图1中,发动机102与TWC系统104机械耦合并流体连通。在TWC系统104中,CC催化剂106与UF催化剂108机械耦合并流体连通。
在一些实施方案中,CC催化剂106体现为包括高PGM载量的PGM商品化催化剂或体现为包括超低PGM载量的SPGM催化剂。在这些实施方案中,UF催化剂108体现为包括高PGM载量的PGM商品化催化剂。由这些实施方案进一步地,发动机102可体现为机动车内所用的内燃机,尤其例如Tier 2bin 4涡轮汽油直喷(TGDI)发动机或自然吸气式进气口喷射(PI)发动机。在这些实施方案中,可以配置各种TWC系统以评估和比较与发动机102一起使用时的催化性能。
TWC系统1
在一些实施方案中,实现TWC系统104,在本文中称为TWC系统1,其包括高PGM基原始设备制造商(OEM)CC和OEM UF催化剂。在这些实施方案中,CC催化剂106是具有大约98g/ft3钯(Pd)和大约8g/ft3铑(Rh)的PGM载量以得出大约106g/ft3的总PGM载量和体积为大约1.7L的基底的高PGM基OEM CC催化剂。由这些实施方案进一步地,UF催化剂108是具有大约51g/ft3Pd和大约8g/ft3Rh的PGM载量以得出大约59g/ft3的总PGM载量和体积为大约1.3L的基底的高PGM基OEM UF催化剂。
TWC系统2
在一些实施方案中,实现TWC系统104,在本文中称为TWC系统2,其包括如上文在TWC系统1中所述的高PGM基OEM UF催化剂和具有超低PGM载量的SPGM CC催化剂。在这些实施方案中,CC催化剂106是SPGM CC催化剂,其包括尖晶石基ZPGM层,被大约5g/ft3铂(Pt)和大约5g/ft3Rh的超低PGM层涂布以得出大约10g/ft3的总PGM载量。
TWC系统3
在一些实施方案中,实现TWC系统104,在本文中称为TWC系统3,其包括市售高PGM基CC和UF催化剂。在这些实施方案中,CC催化剂106是具有大约55.9g/ft3Pd和大约4.3g/ft3Rh的PGM载量以得出大约60.2g/ft3的总PGM载量和体积为大约1.083L的基底的高PGM基CC催化剂。由这些实施方案进一步地,UF催化剂108是具有大约18g/ft3Pt和大约4g/ft3Rh的PGM载量以得出大约22g/ft3的总PGM载量和体积为大约1.083L的基底的高PGM基UF催化剂。
TWC系统4
在一些实施方案中,实现TWC系统104,在本文中称为TWC系统4,其包括PGM基UF催化剂和如上文在TWC系统2中所述的具有超低PGM载量的SPGM CC催化剂。在这些实施方案中,UF催化剂108是具有大约12g/ft3Pd和大约6g/ft3Rh的PGM载量以得出大约18g/ft3的总PGM载量和大约1.083L的基底的PGM基UF催化剂。由这些实施方案进一步地,CC催化剂106是SPGM CC催化剂,其包括尖晶石基ZPGM层,被大约5g/ft3铂(Pt)和大约5g/ft3Rh的超低PGM层涂布以得出大约10g/ft3的总PGM载量。
在一些实施方案中,TWC系统1和TWC系统2与用于测试上述TWC系统的TGDI发动机机械耦合并流体连通。在另一些实施方案中,TWC系统3和TWC系统4与用于测试上述TWC系统的PI发动机机械耦合并流体连通。
SPGM CC催化剂配置
在一些实施方案中,SPGM CC催化剂包括基底、涂布到基底上的洗涂(WC)层和涂布到WC层上的外覆(OC)涂层。在这些实施方案中,使用PGM组合物作为OC层。由这些实施方案进一步地,使用ZPGM组合物作为WC层。由这些实施方案再进一步地,ZPGM和PGM组合物的不同组合提供SPGM CC催化剂配置内的ZPGM WC层和PGM OC层之间的不同相互作用。
SPGM CC催化剂内所用的ZPGM层的材料组成
在一些实施方案中,WC层内所用的ZPGM组合物包括具有通式AXB3-XO4的二元尖晶石结构,其中X是在大约0.01至大约2.99的范围内的摩尔比变量。在这些实施方案中,A和B尤其可体现为Na、K、Mg、Ca、Sr、Ba、Cr、Mn、Fe、Co、Ni、Cu、Zn、Cd、Al、Ti、Ce、La、Pr、Nd、Sm、In或其混合物。由这些实施方案进一步地,该二元尖晶石结构负载到载体氧化物上。载体氧化物的实例尤其包括氧化铝(Al2O3)、掺杂Al2O3、二氧化锆(ZrO2)、掺杂ZrO2、掺杂Al2O3-ZrO2、TiO2、Nb2O5、SiO2或其混合物。
在一个实例中,WC层内所用的ZPGM组合物体现为镍(Ni)和铁(Fe)的二元尖晶石结构。在这一实例中,该Ni-Fe尖晶石结构使用通式NiXFe3-XO4尖晶石制造,其中X对于Ni0.5Fe2.5O4二元尖晶石结构取大约0.5的值。由这一实例进一步地,该Ni0.5Fe2.5O4二元尖晶石结构负载到掺杂Al2O3-ZrO2载体氧化物粉末上。
在另一些实施方案中,WC层内所用的ZPGM组合物包括具有通式AXBYM3-X-YO4的三元尖晶石结构,其中X是在大约0.01至大约1.99的范围内的不同摩尔比的变量,且Y是在大约0.01至大约1.0的范围内的不同摩尔比的变量。在这些实施方案中,A、B和M尤其可体现为Na、K、Mg、Ca、Sr、Ba、Cr、Mn、Fe、Co、Ni、Cu、Zn、Cd、Al、Ti、Ce、La、In或其混合物。由这些实施方案进一步地,该三元尖晶石结构负载到载体氧化物上。载体氧化物的实例尤其包括氧化铝(Al2O3)、掺杂Al2O3、二氧化锆(ZrO2)、掺杂ZrO2、掺杂Al2O3-ZrO2、TiO2、Nb2O5、SiO2或其混合物。
SPGM CC催化剂内所用的PGM层的材料组成
在一些实施方案中,OC层内所用的PGM组合物包括铂(Pt)、钯(Pd)、钌(Ru)、铱(Ir)和铑(Rh),独自或为使用不同载量的它们的组合。在这些实施方案中,该PGM组合物包括负载到载体氧化物上的具有在大约1g/ft3至大约10g/ft3的范围内的基本类似载量的Pt/Rh。在一个实例中,OC层内所用的PGM组合物包括负载到掺杂氧化铝载体氧化物粉末上的大约5g/ft3Pt和大约5g/ft3Rh的PGM载量。
SPGM CC催化剂配置和制造
图2是图解根据一个实施方案的用于CC用途的协同PGM(SPGM)催化剂的催化剂配置的图示。在图2中,催化剂配置200包括基底202、ZPGMWC层204和PGM OC层206。在一些实施方案中,将ZPGM WC层204涂布到基底202上。在这些实施方案中,将PGM OC层206涂布到ZPGMWC层204上。
在一些实施方案中,ZPGM层可使用任何传统催化剂合成方法制造。在这些实施方案中,ZPGM层由包含Ni-Fe尖晶石和掺杂Al2O3-ZrO2的粉末制造。由这些实施方案进一步地,粉状Ni-Fe尖晶石和载体氧化物的制备开始于以产生Ni0.5Fe2.5O4的适当摩尔比混合适当量的硝酸镍溶液和硝酸铁溶液。由这些实施方案再进一步地,经由初湿(IW)法将Ni-Fe硝酸盐溶液逐滴添加到掺杂Al2O3-ZrO2(氧化铝-二氧化锆)载体氧化物粉末中。在这些实施方案中,该Ni-Fe/掺杂Al2O3-ZrO2载体氧化物粉末随后在大约120℃下干燥整夜并在大约600℃至大约850℃范围内的温度下进一步煅烧大约5小时。由这些实施方案进一步地,随后将Ni-Fe二元尖晶石和掺杂Al2O3-ZrO2的煅烧材料研磨成细粒粉末,并进一步用水研磨以制造浆料。由这些实施方案再进一步地,将所述浆料涂布到基底上并进一步干燥和在大约650℃的温度下煅烧大约4小时至大约5小时以产生ZPGM WC层204。
在一个实例中,制造并入TWC系统2和4内的具有超低PGM载量的SPGM CC催化剂,其包括陶瓷基底,例如具有103.0mm的直径(D)和130.0mm的长度(L)的600/3.5 1.083L基底。由这一实例进一步地,该SPGM CC催化剂包括如上所述的包含Ni-Fe二元尖晶石结构和掺杂Al2O3-ZrO2载体氧化物的ZPGM WC层和包含Pt和Rh的PGM OC层。在这一实例中,PGM OC层的制造开始于包括大约5g/ft3Pt和大约5g/ft3Rh的PGM载量的硝酸铂和硝酸铑的混合溶液的制备。由这一实例进一步地,单独研磨掺杂氧化铝(Al2O3)和Ce基储氧材料(OSM)的大约1:1重量比的混合物并用Pt-Rh混合硝酸盐溶液金属化以制造PGM/(掺杂氧化铝+Ce基OSM)的浆料。由这一实例再进一步地,将PGM/(掺杂氧化铝+Ce基OSM)的浆料涂布到ZPGM WC层上,并进一步干燥和在大约550℃的温度下煅烧大约4小时以产生具有超低PGM载量的SPGM CC催化剂。
多模式老化循环程序
在一些实施方案中和在根据FTP-75的排放测试之前,在TWC系统1、2、3和4内的上述CC和UF催化剂在发动机台架上在标准多模式老化循环下老化。在这些实施方案中,CC(PGM基和SPGM)催化剂在多模式老化条件下在大约1000℃的床温度下老化大约50小时。由这些实施方案进一步地,UF催化剂在多模式条件下在大约900℃的床温度下老化大约50小时。
图3是图解根据一个实施方案用于SPGM CC催化剂的发动机台架老化的标准多模式老化循环规程的图示。在图3中,多模式老化循环300图解上述SPGM CC催化剂的老化程序。
在一些实施方案中,多模式老化循环程序包括四段。在这些实施方案中,老化段1使用具有化学计量空气-燃料比(AFR)和每催化转化器大约80SCFM(标准立方英尺/分钟)的流速的排气流进行大约40秒的持续时间。由这些实施方案进一步地,老化段2使用具有富AFR和大约80SCFM流速的排气流进行大约6秒的持续时间。由这些实施方案再进一步地,老化段3使用具有富AFR的排气流和进一步使用二次空气喷射流进行大约10秒的持续时间,由此产生化学反应诱发的热漂移(放热),其具有在大约40mm下控制在大约900℃(在±20℃内)的brick温度。在这些实施方案中,老化段4使用具有化学计量AFR的排气流和进一步使用二次空气喷射流进行大约4秒的持续时间。
U.S.Federal Test Procedure(FTP-75)
图4是图解根据一个实施方案用于测试、测量和诊断如图1和2中所述的TWC系统的催化性能的U.S.Federal Test Procedure(FTP-75)的行驶阶段的图示。在图4中,FTP-75规程400包括冷启动阶段402、稳定化阶段404和热启动阶段406。
在一些实施方案中,冷启动阶段402图解用于测量上述TWC系统的尾管排放和性能的FTP-75测试的一个阶段。在这些实施方案中,所述行驶阶段是进行0至505秒的持续时间的在大约20℃至大约30℃的环境温度下的冷启动短暂阶段。由这些实施方案进一步地,稳定化阶段404图解在冷启动阶段402后进行的大约506秒至大约1372秒的行驶条件的阶段。由这些实施方案再进一步地和在稳定化阶段404结束后,发动机停止大约10分钟,然后开始热启动阶段406。在这些实施方案中,热启动阶段406图解如下在稳定化阶段404后进行的行驶条件的两段:(1)进行大约540秒的最小持续时间或大约660秒的最大持续时间的热浸(hot soak),和(2)进行0至大约505秒的持续时间的热启动短暂阶段。由这些实施方案进一步地,将来自各阶段的尾管排放物收集在单独袋中,分析并以克/英里表示。
用于实施FTP-75试验的试验发动机和发动机规格
在一些实施方案中和参考图1,发动机102体现为具有电子控制的双涡旋涡轮增压器的TGDI发动机,具有连续可变气门正时的双顶置凸轮轴(DOHC)发动机,其中使用凸轮驱动的高压燃料泵进行直接喷射。在这些实施方案中,TGDI发动机包括两级变排量油泵、空气-空气中间冷却系统和铸铝发动机缸体。TGDI发动机的主要规格显示在下表1中。
表1.TGDI发动机规格
规格 | 单位 | 值 |
排量 | cm<sup>3</sup> | 1,998.0 |
压缩比 | 9.5:1 | |
最大扭矩 | lb-ft | 295.0@3,000-4,000rpm |
功率 | HP | 259.0 |
在另一些实施方案中和参考图1,发动机102体现为具有压铸铝发动机缸体(具有16个双可变气门正时(VVT-i)的气门)的PI发动机,包括偏置曲轴和具有滚轮摇臂的气门机构、三级变量油泵、低张力活塞环和辅助皮带驱动的低摩擦技术。在这些实施方案中,PI发动机包括声控进气系统,其基于RPM和节气门角度转变两个阶段之间的进气道的长度,以确保在宽发动机速度范围间的强扭矩。由这些实施方案进一步地,PI发动机包括新型tumblecontrol阀,其在发动机冷的同时增强燃烧并有助于使催化转化器迅速达到工作温度。由这些实施方案再进一步地,tumble control阀与新型12孔高雾化长喷嘴燃料喷射器一起减少附着到进气口的燃料量以使燃料经济性最大化和减少有害排放物。PI发动机的主要规格显示在下表2中。
表2.PI发动机规格
规格 | 单位 | 值 |
排量 | cm<sup>3</sup> | 2,494.0 |
压缩比 | 10.4:1 | |
最大扭矩 | lb-ft | 170.0@4,100rpm |
功率 | HP | 178.0 |
来自FTP-75试验-TGDI发动机的尾管加权排放袋结果
图5是图解根据一个实施方案使用如图4中所述的FTP-75试验规程的涡轮汽油直喷(TGDI)发动机内所用的TWC系统1和2(如上所述)的尾管处加权NOX(克/英里)值的图示。在图5中,TP加权NOX排放500包括TWC系统1TP加权NOX 502和TWC系统2TP加权NOX 510。
在一些实施方案中,TWC系统1TP加权NOx 502包括下列三个具体TP加权NOX条:TP加权NOx条504、TP加权NOx条506和TP加权NOx条508。在这些实施方案中,各NOX条分别图解在测量与TWC系统1相关的尾管NOx排放时获得的冷启动阶段402、稳定化阶段404和热启动阶段406的加权NOX的以克/英里计的FTP-75袋结果。在另一些实施方案中,TWC系统2TP NOX加权510包括下列三个具体TP加权NOX条:TP加权NOx条512、TP加权NOx条514和TP加权NOx条516。在这些实施方案中,各NOX条分别图解在测量与TWC系统2相关的尾管NOX排放时获得的冷启动阶段402、稳定化阶段404和热启动阶段406的加权NOX的以克/英里计的FTP-75袋结果。
在一些实施方案中,在与TWC系统1和2相关的FTP-75测试的实施过程中以克/英里为单位收集的TP加权NOX排放详列在下表3中。在这些实施方案中,TWC系统2包括具有超低PGM载量的SPGM CC和OEMUF催化剂,其表现出比包括OEM CC和UF催化剂的TWC系统1低的尾管(TP)加权NOX值。由这些实施方案进一步地,TWC系统2表现出比TWC系统1高效的TP NOX转化。由这些实施方案再进一步地和在冷启动阶段402结束时,TWC系统1表现出比TWC系统2高的TP加权NOX值。在这些实施方案中,这两个上述TWC系统表现出基本类似的稳定化阶段404和热启动阶段406的TP加权NOX值。概括而言,TWC系统2表现出与TWC系统1相比略微改进的NOX还原性能,由此证实使用具有超低PGM载量的SPGM CC与使用高PGM商品化CC催化剂一样有效。
表3.如图5中所示与TWC系统1和2相关的TP加权NOX排放值
FTP-75阶段 | TWC系统 | TP加权NOx[克/英里] | 相关元素 |
冷启动阶段402 | 1 | 0.033 | 504 |
稳定化阶段404 | 1 | 0.001 | 506 |
热启动阶段406 | 1 | 0.005 | 508 |
冷启动阶段402 | 2 | 0.027 | 512 |
稳定化阶段404 | 2 | 0.001 | 514 |
热启动阶段406 | 2 | 0.006 | 516 |
图6是图解根据一个实施方案使用如图4中所述的FTP-75试验规程TGDI发动机内所用的TWC系统1和2(如上所述)的尾管处加权CO(克/英里)值的图示。在图6中,TP加权CO排放600包括TWC系统1TP加权CO 602和TWC系统2TP加权CO 610。
在一些实施方案中,TWC系统1TP加权CO 602包括下列三个具体加权CO条:TP加权CO条604、TP加权CO条606和TP加权CO条608。在这些实施方案中,各CO条分别图解在测量与TWC系统1相关的尾管CO排放时获得的冷启动阶段402、稳定化阶段404和热启动阶段406的加权CO的以克/英里计的FTP-75袋结果。在另一些实施方案中,TWC系统2TP加权CO 610包括下列三个具体加权CO条:TP加权CO条612、TP加权CO条614和TP加权CO条616。在这些实施方案中,各CO条分别图解在测量与TWC系统2相关的尾管CO排放时获得的冷启动阶段402、稳定化阶段404和热启动阶段406的加权CO的以克/英里计的FTP-75袋结果。
在一些实施方案中,在与TWC系统1和2相关的FTP-75测试的实施过程中以克/英里为单位收集的TP加权CO排放详列在下表4中。在这些实施方案中,TWC系统2包括具有超低PGM载量的SPGM CC催化剂,其与包括OEM CC和UF催化剂的TWC系统1相比表现出整体显著的CO转化。由这些实施方案进一步地,TWC系统2表现出比TWC系统1高效的CO转化。由这些实施方案再进一步地,对于冷启动阶段402、稳定化阶段404和热启动阶段406,TWC系统2的TP加权CO值明显低于TWC系统1的TP加权CO值。这些结果证实,对于CO转化,使用具有大约10g/ft3PGM载量的SPGM CC催化剂与使用具有大约106g/ft3PGM载量的高PGM OEM CC催化剂一样有效。
表4.如图6中所示与TWC系统1和2相关的TP加权CO排放值
FTP-75阶段 | WC系统 | TP加权CO[克/英里] | 相关元素 |
冷启动阶段402 | 1 | 0.270 | 604 |
稳定化阶段404 | 1 | 0.441 | 606 |
热启动阶段406 | 1 | 0.458 | 608 |
冷启动阶段402 | 2 | 0.197 | 612 |
稳定化阶段404 | 2 | 0.297 | 614 |
热启动阶段406 | 2 | 0.200 | 616 |
图7是图解根据一个实施方案使用如图4中所述的FTP-75试验规程TGDI发动机内所用的TWC系统1和2(如上所述)的尾管处加权THC(克/英里)值的图示。在图7中,TP加权THC排放700包括TWC系统1TP加权THC 702和TWC系统2TP加权THC 710。
在一些实施方案中,TWC系统1TP加权THC 702包括下列三个具体TP加权THC条:TP加权THC条704、TP加权THC条706和TP加权THC条708。在这些实施方案中,各THC条分别图解在测量与TWC系统1相关的尾管THC排放时获得的冷启动阶段402、稳定化阶段404和热启动阶段406的加权THC的以克/英里计的FTP-75袋结果。在另一些实施方案中,TWC系统2TP加权THC 710包括下列三个具体TP加权THC条:TP加权THC条712、TP加权THC条714和TP加权THC条716。在这些实施方案中,各THC条分别图解在测量与TWC系统2相关的尾管THC排放时获得的冷启动阶段402、稳定化阶段404和热启动阶段406的加权THC的以克/英里计的FTP-75袋结果。
在一些实施方案中,在与TWC系统1和2相关的FTP-75测试的实施过程中以克/英里为单位收集的TP加权THC排放详列在下表5中。在这些实施方案中,TWC系统2包括具有超低PGM载量的SPGM CC催化剂,其表现出比包括OEM CC和UF催化剂的TWC系统1高的TP加权THC值。由这些实施方案进一步地,TWC系统2表现出比TWC系统1低的THC转化性能。
表5.如图7中所示与TWC系统1和2相关的TP加权THC排放值
FTP-75阶段 | WC系统 | TP加权THC[克/英里] | 相关元素 |
冷启动阶段402 | 1 | 0.028 | 704 |
稳定化阶段404 | 1 | 0.005 | 706 |
热启动阶段406 | 1 | 0.005 | 708 |
冷启动阶段402 | 2 | 0.045 | 712 |
稳定化阶段404 | 2 | 0.012 | 714 |
热启动阶段406 | 2 | 0.012 | 716 |
图8是图解根据一个实施方案使用如图4中所述的FTP-75试验规程TGDI发动机内所用的TWC系统1和2(如上所述)的尾管处加权非甲烷烃(NMHC)(克/英里)值的图示。在图8中,TP加权NMHC排放800包括TWC系统1TP加权NMHC 802和TWC系统2TP加权NMHC 810。
在一些实施方案中,TWC系统1TP加权NMHC 802包括下列三个具体TP加权NMHC条:TP加权NMHC条804、TP加权NMHC条806和TP加权NMHC条808。在这些实施方案中,各NMHC条分别图解在测量与TWC系统1相关的尾管NMHC排放时获得的冷启动阶段402、稳定化阶段404和热启动阶段406的加权NMHC的以克/英里计的FTP-75袋结果。在另一些实施方案中,TWC系统2TP加权NMHC 810包括下列三个具体NMHC TP加权条:TP加权NMHC条812、TP加权NMHC条814和TP加权NMHC条816。在这些实施方案中,各NMHC条分别图解在测量与TWC系统2相关的尾管NMHC排放时获得的冷启动阶段402、稳定化阶段404和热启动阶段406的加权NMHC的以克/英里计的FTP-75袋结果。
在一些实施方案中,在与TWC系统1和2相关的FTP-75测试的实施过程中以克/英里为单位收集的TP加权NMHC排放详列在下表6中。在这些实施方案中,TWC系统2包括具有超低PGM载量的SPGM CC催化剂,其表现出比包括OEM CC和UF催化剂的TWC系统1略高的TP加权NMHC值。概括而言,TWC系统2在FTP-75的各个阶段的过程中表现出的催化行为与高PGM基OEM催化剂的催化行为相当。
表6.如图7中所示与TWC系统1和2相关的TP加权NMHC排放值
FTP-75阶段 | WC系统 | TP加权NMHC[克/英里] | 相关元素 |
冷启动阶段402 | 1 | 0.022 | 804 |
稳定化阶段404 | 1 | 0.002 | 806 |
热启动阶段406 | 1 | 0.002 | 808 |
冷启动阶段402 | 2 | 0.035 | 812 |
稳定化阶段404 | 2 | 0.003 | 814 |
热启动阶段406 | 2 | 0.005 | 816 |
图9是图解根据一个实施方案TWC系统1和2(如上所述)和使用在给定速度下的TGDI发动机的累积中尾管NOX排放结果的图示。在图9中,累积NOX值比较900包括累积NOX曲线902、累积NOX曲线904和FTP-75规程400。在图9中,具有与上图基本类似的元素号的元素以基本类似的方式运作。
在一些实施方案中,累积NOX曲线902显示在给定速度下与TWC系统1相关的在中尾管(MID)处获得的累积NOX排放结果。在这些实施方案中,累积NOX曲线904显示在给定速度下与TWC系统2相关的在MID处获得的累积NOX排放结果。
在一些实施方案中,对于TWC系统1和2,在Federal Test Procedure(FTP-75)规程,如图4中所述的FTP-75规程400的实施过程中获得结果。在这些实施方案中,比较各TWC系统的结果以评估包括SPGM CC催化剂的TWC系统的转化效率和性能的改进。由这些实施方案进一步地,证实上述SPGM CC催化剂对NOX的协同效应。在这些实施方案中,通过比较在给定速度下在包括如上所述的TGDI发动机的发动机排气系统的中尾管段下游测得的TWC系统1和2的累积NOX克数,进行协同效应的核实。
在一些实施方案中,与TWC系统2相关的累积MID NOX值(累积NOX曲线904)明显低于与TWC系统1相关的累积MID NOX值(累积NOX曲线902)。在这些实施方案中,NOx中尾管排放的改进(累积NOX曲线904)表明SPGM CC催化剂表现出比OEM PGM CC催化剂高的功能性。由这些实施方案进一步地,SPGM CC催化剂内的尖晶石氧化物ZPGM层增强PGM层的功能性,由此降低与TWC系统2相关的NOx中尾管排放值。概括而言,TWC系统2表现出比TWC系统1高的NOX转化效率。
图10是图解根据一个实施方案TWC系统1和2(如上所述)和使用在给定速度下的TGDI发动机的累积中尾管THC排放结果的图示。在图10中,累积THC值比较1000包括累积THC曲线1002、累积THC曲线1004和FTP-75规程400。在图10中,具有与上图基本类似的元素号的元素以基本类似的方式运作。
在一些实施方案中,累积THC曲线1002显示与TWC系统1相关的在中尾管(MID)处获得的累积THC排放结果。在这些实施方案中,累积THC曲线1004显示与TWC系统2相关的在MID处获得的累积THC排放结果。
在一些实施方案中,对于TWC系统1和2,在Federal Test Procedure(FTP-75)规程,如图4中所述的FTP-75规程400的实施过程中获得结果。在这些实施方案中,比较各TWC系统的结果以评估包括超低载量SPGMCC催化剂的TWC系统的转化效率和性能的改进。由这些实施方案进一步地,证实上述SPGM CC催化剂对THC的协同效应。在这些实施方案中,通过比较在给定速度下在包括如上所述的TGDI发动机的发动机排气系统的中尾管段下游测得的TWC系统1和2的累积THC克数,进行协同效应的核实。
在一些实施方案中,与TWC系统2相关的累积MID NOX值(累积NOX曲线1004)略高于与TWC系统1相关的累积MID NOX值(累积NOX曲线902)。概括而言,TWC系统2表现出比TWC系统1略低的THC转化效率。
来自FTP-75试验-PI发动机的尾管加权排放袋结果
图11是图解根据一个实施方案使用如图4中所述的FTP-75试验规程自然吸气式进气口喷射(PI)发动机内所用的TWC系统3和4(如上所述)的尾管处加权NOX(克/英里)值的图示。在图11中,TP加权NOX排放1100包括TWC系统3TP加权NOX 1102和TWC系统4TP加权NOX1110。
在一些实施方案中,TWC系统3TP加权NOX 1102包括下列三个具体TP加权NOX条:TP加权NOx条1104、TP加权NOx条1106和TP加权NOx条1108。在这些实施方案中,各NOX条分别图解在测量与TWC系统3相关的尾管NOx加权排放时获得的冷启动阶段402、稳定化阶段404和热启动阶段406的加权NOX的以克/英里计的FTP-75袋结果。在另一些实施方案中,TWC系统4TP NOX加权1110包括下列三个具体TP加权NOX条:TP加权NOx条1112、TP加权NOx条1114和TP加权NOx条1116。在这些实施方案中,各NOX条分别图解在测量与TWC系统4相关的尾管NOX排放时获得的冷启动阶段402、稳定化阶段404和热启动阶段406的加权NOX的以克/英里计的FTP-75袋结果。
在一些实施方案中,在与TWC系统3和4相关的FTP-75测试的实施过程中以克/英里为单位收集的TP加权NOX排放详列在下表7中。在这些实施方案中,TWC系统4包括SPGM CC和PGM基UF催化剂,其表现出比包括OEM CC和UF催化剂的TWC系统3高的NOX转化。由这些实施方案进一步地和在冷启动阶段402结束时,TWC系统4表现出比TWC系统3略高的TP加权NOX值。由这些实施方案再进一步地和在稳定化阶段404和热启动阶段406之后,TWC系统4表现出比TWC系统3低的TP加权NOX值。这些结果证实,使用结合Ni-Fe二元尖晶石至低载量PGM(总计10g/ft3)的SPGM CC催化剂是有效的CC催化剂。概括而言,与TWC系统3相比,TWC系统4表现出改进的NOX还原性能。
表7.如图11中所示与TWC系统3和4相关的TP加权NOX排放值
FTP-75阶段 | TWC系统 | TP加权NOx[克/英里] | 相关元素 |
冷启动阶段402 | 3 | 0.013 | 1104 |
稳定化阶段404 | 3 | 0.006 | 1106 |
热启动阶段406 | 3 | 0.002 | 1108 |
冷启动阶段402 | 4 | 0.015 | 1112 |
稳定化阶段404 | 4 | 0.003 | 1114 |
热启动阶段406 | 4 | 0.001 | 1116 |
尽管已经公开了各种方面和实施方案,但可能想出其它方面和实施方案。本文中公开的各种方面和实施方案用于举例说明并且无意构成限制,由下列权利要求书指示真实范围和精神。
Claims (20)
1.一种用于处理内燃机的排气料流的催化系统,其包含
内燃机;
配置成接收来自所述内燃机的至少一个排气料流的紧耦合催化转化器,所述紧耦合催化转化器包含含有零铂族金属尖晶石催化剂组合物和超低铂族金属催化剂材料的协同铂族金属催化剂,其中所述铂族金属催化剂材料具有大约1g/ft3至大约10g/ft3的铂族金属浓度;和
在所述紧耦合催化转化器下游并与其流体连通的地板下催化转化器,所述地板下催化转化器包含铂族金属催化剂。
2.权利要求1的催化系统,其中所述地板下催化转化器具有大约10至100g/ft3的铂族金属浓度。
3.权利要求1的催化系统,其中所述地板下催化转化器的铂族金属选自铂、钯、钌、铱和铑。
4.权利要求3的催化系统,其中所述地板下催化转化器的铂族金属包含铂和铑的组合。
5.权利要求1的催化系统,其中所述尖晶石催化剂组合物包含具有通式AxB3-xO4的二元尖晶石,其中X为0.01至2.99,且A和B选自钠、钾、钙、钡、锌、镉、铝、镁、锰、镍、铜、钴、铁、铬、钛、铈、锶、镧、镨、钕、钐、铟及其混合物。
6.权利要求5的催化系统,其中所述二元尖晶石包含Ni-Fe尖晶石。
7.权利要求6的催化系统,其中所述Ni-Fe尖晶石包含Ni0.5Fe2.5O4。
8.权利要求1的催化系统,其中所述尖晶石催化剂组合物包含至少一种基底,和含有具有式AXBYM3-X-Y的尖晶石氧化物的催化剂组合物,其中X为大约0.01至大约1.99且Y为大约0.01至大约1.0,且其中A、B和M彼此不同并选自钠、钾、钙、钡、锌、镉、铝、镁、锰、镍、铜、钴、铁、铬、钛、铈、锶、镧、镨、钕、钐、铟及其混合物。
9.权利要求1的催化系统,其中所述尖晶石催化剂组合物负载到选自Al2O3、掺杂Al2O3、ZrO2、掺杂ZrO2、SiO2、掺杂SiO2、TiO2、掺杂TiO2、掺杂Al2O3-ZrO2、Nb2O5及其混合物的载体氧化物上。
10.权利要求1的催化系统,其中所述尖晶石催化剂组合物作为洗涂层沉积到基底上,且所述超低铂族金属催化剂材料作为外覆涂层沉积到所述洗涂层上。
11.权利要求1的催化系统,其中所述超低铂族金属催化剂的铂族金属选自铂、钯、钌、铱和铑。
12.权利要求1的催化系统,其中所述超低铂族金属催化剂的铂族金属包含铂和铑的组合。
13.权利要求1的催化系统,其中所述超低铂族金属催化剂材料中的铂量为大约1至5g/ft3,且所述超低铂族金属催化剂材料中的铑量为大约1至5g/ft3。
14.权利要求13的催化系统,其中所述超低铂族金属催化剂材料的铂和铑以1:1比率存在。
15.权利要求1的催化系统,其中所述尖晶石催化剂组合物包含负载到掺杂Al2O3-ZrO2载体氧化物上的Ni-Fe二元尖晶石结构。
16.权利要求1的催化系统,其中所述地板下催化转化器包含铂和铑的组合,且其中所述地板下催化转化器中的铂族金属总量为大约15至25g/ft3。
17.权利要求1的催化系统,其中所述协同铂族金属催化剂的铂族金属催化剂不含稀土金属和储氧材料。
18.权利要求1的催化系统,其中所述催化系统表现出与具有铂族金属催化剂代替所述协同铂族金属催化剂作为紧耦合催化转化器的类似系统相比NOx、CO和THC的尾管排放的降低。
19.一种从内燃机排气料流中除去污染物的方法,其包含
将内燃机排气料流引入包含含有零铂族金属尖晶石催化剂组合物和超低铂族金属催化剂材料的协同铂族金属催化剂的紧耦合催化转化器,其中所述铂族金属催化剂具有大约1g/ft3至大约10g/ft3的浓度由此至少部分催化转化NOx、CO和THC;
将所述至少部分催化转化的排气料流引入包含铂族金属催化剂的地板下催化转化器。
20.权利要求19的方法,其中所述尖晶石催化剂组合物包含负载到掺杂Al2O3-ZrO2载体氧化物上的Ni-Fe二元尖晶石结构。
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