CN101970088B - 催化烟灰过滤器的制造和系统 - Google Patents
催化烟灰过滤器的制造和系统 Download PDFInfo
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- CN101970088B CN101970088B CN2008801218020A CN200880121802A CN101970088B CN 101970088 B CN101970088 B CN 101970088B CN 2008801218020 A CN2008801218020 A CN 2008801218020A CN 200880121802 A CN200880121802 A CN 200880121802A CN 101970088 B CN101970088 B CN 101970088B
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Abstract
壁流块料蜂窝式过滤器具有包括平均宽度小于0.4μm的微裂纹,和平均孔尺寸为10μm~25μm的孔;和在壁流块料的壁内设置的涂层,所述涂层包括含有载体颗粒和至少一种贵金属的催化剂,其中至少90%的载体颗粒具有大于微裂纹的平均尺寸的颗粒度并且至少90%的载体颗粒具有小于壁流块料的孔的平均尺寸的颗粒度。壁流块料包含孔隙度为40%~70%的钛酸铝,其中当在1000℃测量时烟灰过滤器显示热膨胀系数小于25×10-7/K,当在800℃测量时优选小于5×10-7/K。
Description
相关申请的交叉引用
本申请是2007年12月18日递交的美国专利申请系列号11/959,090的部分继续申请,其全部内容引入本文供参考。
技术领域
公开了用于柴油机废气排放系统的催化烟灰过滤器及其制造方法和用途。
背景技术
柴油机废气是多相混合物,不仅含有气体排放物,例如一氧化碳(“CO”)、未燃烧的烃(“HC”)和氮氧化物(“NOx”),还含有构成所谓的微粒或颗粒物质的冷凝相材料(液体和固体)。通常,在柴油机排气系统中提供催化剂组合物和负载这些组合物的基底,以便将某些或所有这些废气组分转化为无害组分。例如,柴油机排气系统可以包含一种或多种柴油机氧化催化剂、烟灰过滤器和用于还原NOx的催化剂。
已知含有铂族金属、基底金属及其组合的氧化催化剂通过促进HC和CO两种气体污染物和一部分颗粒物质通过这些污染物的氧化而转化成二氧化碳和水而有助于柴油机废气的处理。这种催化剂通常包含在被置于柴油机废气中以便在废气排入大气之前对其进行处理的被称为柴油机氧化催化剂(DOC)的单元中。除了气体HC、CO和颗粒物质的转化,含有铂族金属的氧化催化剂(其通常分散在难熔氧化物载体上)还促进了将一氧化氮(NO)转化为NO2的氧化。柴油机废气的总颗粒物质排放物由三种主要组分组成。一种组分是固态、干燥的、固体含碳部分或烟灰部分。这种干燥含碳物质有助于通常与柴油机废气相联系的可见烟灰排放物。颗粒物质的第二组分是可溶有机部份(“SOF”)。可溶有机部份有时称为挥发分有机部份(“VOF”),本文中将使用该术语。取决于柴油机废气的温度,VOF可以以蒸气或气溶胶(小液滴冷凝物)而存在于柴油机废气中。如标准测量试验,例如U.S.Heavy Duty Transient Federal Test Procedure所规定,在52℃的标准微粒收集温度下,其通常以冷凝液体存在于稀释的废气中。这些液体来自两个来源:(1)活塞每次上下时从发动机的汽缸壁扫下的润滑油;和(2)未燃烧的或部分燃烧的柴油。
颗粒物质的第三种组分是所谓的硫酸盐部分。这种硫酸盐部分是由柴油燃料中存在的少量硫组分形成的。在柴油燃烧过程中形成小比例的SO3,接着其又迅速与废气中的水结合形成硫酸。硫酸作为凝相与气溶胶形式的颗粒一起汇集,或者被吸附到其它颗粒组分上,并从而添加了TPM的质量。
用于高度减少颗粒物质的一种关键的后处理技术是柴油机微粒过滤器。有许多已知的从柴油机废气中有效去除颗粒物质的过滤器结构,例如蜂窝壁流过滤器、缠绕的或装填的纤维过滤器、开放孔隙泡沫烧结金属过滤器等。然而,下述陶瓷壁流过滤器收到最多关注。这些过滤器能够去除柴油机废气中超过90%的颗粒物质。过滤器是用于从废气中去除颗粒的物理结构,且聚积的颗粒会增加过滤器对发动机的背压。因此,聚积的颗粒必须连续或定期从过滤器中烧除以保持可接受的背压。遗憾地是,炭黑颗粒需要超过500℃的温度以便在富氧(贫)废气条件下燃烧。这一温度高于柴油机废气中通常存在的温度。
通常提供条件降低烟灰燃烧温度以便提供过滤器的被动再生。催化剂的存在促进了烟灰燃烧,由此在实际载荷循环下在柴油机废气中可以达到的温度下使过滤器再生。用这种方法,催化烟灰过滤器(CSF)或催化柴油机微粒过滤器(CDPF)能够在聚积的烟灰被动燃烧的同时有效地减少>80%的颗粒物质,并由此促进过滤器再生。
用于在钛酸铝和堇青石基底上的涂布柴油机微粒过滤器的常规方法,与未涂布的过滤器相比往往消极地影响涂布过滤器的物理性能。相信在涂层过程中可溶和精细颗粒进入微裂纹中。因此,微裂纹中的材料限制微裂纹的自由运动且降低加热时过滤器膨胀的挠性。为了将这个问题降至最低,在涂层基底前采用聚合物钝化步骤。这种聚合物钝化步骤的实例记载在美国专利号7,166,555中。这一聚合物钝化步骤提高了制造成本和复杂性。因而,希望提供用于在涂层前无需聚合物钝化的制造催化烟灰过滤器的方法。
概述
本文公开了催化烟灰过滤器、用于制造它们的方法和用途以及引入催化烟灰过滤器的系统。在一个实施方案中,催化烟灰过滤器包括壁流块料,其具有多个由纵向延伸壁形成的纵向延伸通道,纵向延伸壁划定所述通道的边界并限定所述通道,通道包括具有开放的入口端和封闭的出口端的入口通道,和具有封闭的入口端和开放的出口端的出口通道,壁流块料包含平均宽度小于约0.4μm的微裂纹,和平均孔尺寸为约10μm~约25μm的孔;以及在壁流块料的壁内设置的涂层,所述涂层包括含有载体颗粒和至少一种贵金属的催化剂,其中至少约90%的载体颗粒具有大于微裂纹的大约平均尺寸的颗粒度并且至少约90%的载体颗粒具有小于壁流块料的孔的大约平均尺寸的颗粒度。
本发明的另一方面涉及制备包含平均宽度小于约0.4μm的微裂纹和平均孔尺寸为约10μm~约25μm的孔的催化剂涂布的壁流块料的方法,该方法包括提供壁流块料,其具有多个由纵向延伸壁形成的纵向延伸通道,纵向延伸壁划定所述通道的边界并限定所述通道,通道包括具有开放的入口端和封闭的出口端的入口通道,和具有封闭的入口端和开放的出口端的出口通道,以及用包含可热分解的催化材料和固体颗粒的含水浆料的形式的涂层涂布壁流块料,至少约90%的颗粒具有大于微裂纹的大约平均尺寸的颗粒度,且至少约90%的颗粒具有小于孔的大约平均尺寸的颗粒度;以及将涂布的壁流块料加热至足够干燥涂层的温度。
附图的简要说明
图1显示排放处理系统的实施方案的示意图;
图2显示壁流过滤器基底的透视图;
图3显示壁流过滤器基底部分的剖视图;
图4显示示例性的壁流基底的热膨胀系数的图;
图5显示机械分离至含有不同程度精细物的喷射研磨的颗粒度分布图;
图6显示用图5中喷射研磨的氧化铝粉末涂布的烟灰过滤器的热膨胀系数的图;
图7显示湿磨和干磨颗粒之间的颗粒度分布;
图8显示通过湿磨和干磨方法制备的烟灰过滤器的热膨胀系数的比较图;和
图9显示通过湿磨和干磨方法制备的过滤器的催化性能的比较图。
详细说明
在描述本发明的几个示例性的实施方案之前,要理解的是,本发明不限制于下列说明中阐述的构造或工艺步骤的细节。本发明能够以各种方式实施或进行。
除非上下文另外清楚地指明,在说明书和所附权利要求中所使用的单数形式“一”和“该”等包括复数对象。因此,例如参考“一种催化剂”包括两种或更多种催化剂的混合物等。
本发明的一方面涉及烟灰过滤器、包括催化烟灰过滤器的柴油机废气处理系统以及制备催化烟灰过滤器的方法。本发明的一个或多个实施方案涉及制备用作排放处理系统部分的催化烟灰过滤器的涂布工艺。
本文提供了将催化剂组合物施用至烟灰过滤器的方法,其中在施用涂层前无需使用聚合物钝化步骤而产生具有优于空白过滤器的物理性能的催化烟灰过滤器。催化烟灰过滤器包括壁流块料和包含催化剂的涂层。壁流块料具有多个由纵向延伸壁形成的纵向延伸通道,纵向延伸壁划定所述通道的边界并限定所述通道。通道包括具有开放的入口端和封闭的出口端的入口通道,和具有封闭的入口端和开放的出口端的出口通道。壁流块料具有平均宽度小于约0.4μm的微裂纹,和平均孔尺寸为约10μm~约25μm的孔;催化剂包含载体颗粒和至少一种贵金属。至少约90%的载体颗粒具有大于微裂纹的大约平均尺寸的颗粒度,并且至少约90%的载体颗粒具有小于壁流块料的孔的大约平均尺寸的颗粒度。
本发明的其它方面涉及制备催化剂涂布的壁流块料的方法,壁流块料包含平均宽度小于约0.4μm的微裂纹和平均孔尺寸为约10μm~约25μm的孔。根据一个或多个实施方案,该方法包括用以含水浆料形式的涂层的壁流块料。含水浆料可包括含有载体颗粒的可热分解的催化材料。载体颗粒以其中至少约90%的颗粒大于微裂纹的大约平均尺寸,并且至少约90%的颗粒小于孔的大约平均尺寸的尺寸范围存在。可将涂布的壁流块料加热至足够在块料表面上提供催化活性化合物的沉积物的温度。
在一些实施方案中,至少约90%的载体颗粒为大于约0.5μm。在详细的实施方案中,载体颗粒为大于约1μm,在更详细的实施方案中,载体颗粒为大于约2μm。在某些实施方案中,至少约90%的载体颗粒为小于约15μm。在特定的实施方案中,载体颗粒为小于约10μm,在更特定的实施方案中,载体颗粒为小于约7.5μm。在最特定的实施方案中,载体颗粒为小于约5μm。在其它实施方案中,多于约60%的载体颗粒为约1μm~约5μm。在另外的实施方案中,多于约75%的载体颗粒为约1μm~约5μm。在其它的实施方案中,多于约80%的载体颗粒为约1μm~约5um。
图1以示意图描绘了排放处理系统的一个实施方案。在图1中可以看出,包含气体污染物(包括未燃烧的烃、一氧化碳和NOx)和颗粒物质的废气从发动机15输送到氧化催化剂11。在氧化催化剂11中,未燃烧的气态和不挥发性烃类(即VOF)和一氧化碳基本燃烧形成二氧化碳和水。使用氧化催化剂除去相当大比例的VOF,特别有助于防止太多颗粒物质沉积在位于该系统下游的烟灰过滤器12上(即阻塞)。此外,在氧化催化剂中,NOx组分的相当大比例的NO氧化为NO2。
将废气流输送到涂布有催化剂组合物的烟灰过滤器12。根据一个或多个实施方案,还通过烟灰过滤器基本去除(超过80%)包含烟灰部分和VOF的颗粒物质。通过过滤器的再生,沉积在烟灰过滤器上的颗粒物质燃烧。置于烟灰过滤器上的催化剂组合物的存在降低了颗粒物质的烟灰部分燃烧时的温度。催化烟灰过滤器12可任选包含SCR催化剂,用于将废气流中的NOx转化为氮气。
可用于负载催化剂组合物的壁流基底具有多个细的、沿基底纵轴延伸的基本平行的气体流动通道。通常,各通道在基底主体一端被堵塞,交替的通道在另一端面被堵塞。这种块料载体可以包含每平方英寸大于约250个孔隙,以及每平方英寸横截面至多约700或更多流动通道(或“孔隙”),尽管可使用远远更少的量。例如,载体可以具有每平方英寸约7~600、更通常约100~400个孔隙(“cpsi”)。孔隙可以具有矩形、正方形、圆形、椭圆形、三角形、六边形或其它多边形的横截面。壁流基底通常具有约0.002~0.1英寸的壁厚。其它实施方案具有约0.002~0.025英寸的壁厚。详细的实施方案具有约0.010英寸~约0.020英寸的壁厚。
图2和3说明具有多个通道52的壁流过滤器基底30。这些通道被过滤器基底的内壁53管状包围。基底具有入口端54和出口端56。交替的通道在入口端被入口塞58堵塞,在出口端被出口塞60堵塞,从而在入口54和出口56处形成相反的棋盘状图案。气流62通过未堵塞的通道入口64进入,被出口塞60挡住,并经由通道壁53(其为多孔的)向出口侧66扩散。由于入口塞58,该气体不能返回壁的入口侧。
某些实施方案的载体颗粒选自铝化合物、锆化合物、铈化合物、沸石、硅化合物、基底金属氧化物及其组合。
壁流过滤器基底,还称为壁流块料和壁流基底,由陶瓷类材料组成,例如堇青石、α-氧化铝、碳化硅、氮化硅、氧化锆、莫来石、锂辉石、氧化铝-二氧化硅-氧化镁或硅酸锆、或多孔耐熔金属。壁流基底还可以由陶瓷纤维复合材料形成。其它实施方案的壁流块料为钛酸铝、堇青石、碳化硅、金属氧化物和陶瓷的一种或多种。
本发明的各种实施方案包括钛酸铝壁流块料,其孔隙率为约40%~约70%。当在1000℃测量时,这一类型的其它实施方案具有小于约25×10-7/℃的热膨胀系数。当在1000℃测量时,更详细的实施方案具有小于约15×10-7/℃的CTE。在其它实施方案中,壁流块料包括选自钛酸铝、堇青石和碳化硅的材料。
根据某些详细的实施方案,当在800℃测量时,烟灰过滤器的热膨胀系数为小于约5×10-7/℃。在其它详细实施方案中,当在800℃测量时,CTE为小于约2×10-7/℃。在其它详细的实施方案中,当在800℃测量时,CTE为小于约1×10-7/℃。
通过将基底垂直浸入一部分催化剂浆料中使得基底顶部刚刚高于浆料表面,获得用催化剂组合物涂布壁流基底。用这样的方式,浆料与各蜂窝壁入口面接触,但是阻止其与各壁的出口面接触。样品在浆料中放置大约30秒。从浆料中去除基底,并如下从壁流基底去除过量浆料:首先将其从通道中排干,然后用压缩空气吹气(与浆料渗透方向相反),然后从浆料渗透方向抽真空。通过使用该技术,催化剂浆料渗透基底壁,然而孔没有堵塞到在最终基底中形成不适当的背压的程度。当用于描述催化剂浆料在基底上的分散时,本文中所用的术语“渗透”是指催化剂组合物在整个基底壁中分散。
通常在约100℃干燥并且在更高的温度(例如300℃~450℃)下锻烧涂布基底。煅烧之后,可通过计算基底涂布和未涂布的重量来测定催化剂负载量。对本领域技术人员显而易见的是,可以通过改变固含量来改性催化剂负载量。或者,可将基底重复浸在涂布浆料中,然后如上所述去除过量浆料。
催化剂分散在合适的载体材料上,例如具有高表面积和良好热稳定性的难熔氧化物,例如高表面积氧化铝。用第二氧化物稳定的氧化铝也是合适的载体。氧化铝的氧化镧稳定化为贵金属催化剂提供合适的载体。氧化铝的混合物也是合适的载体。还可以使用用氧化物如SiO2、ZrO2、TiO2等掺杂或处理的其它氧化铝,以提供稳定化或改进的表面化学。可使用的其它合适的载体材料包括但不限于ZrO2和TiO2,除了上述载体氧化物,经证实可能有用的是包括引入催化区中的其它催化功能的氧化物。这些的实例包括CeO2、Pr6O11、V2O5和MnO2及其组合和固溶体氧化物混合物等。这些氧化物可有助于烃类(特别是重质燃料衍生的烃类)和由注入燃料的歧化(即脱氢或氧化脱氢)生成的沉积的焦炭/烟灰的燃烧,并由此使催化区产生额外的燃烧活性,并防止由烃衍生焦炭的沉积造成的PGM钝化。
实施例
以下实施例进一步说明本发明,而是当然不应该认为是以任何方式限制其保护范围。例如,当实施例提供钛酸铝和堇青石壁流过滤器,可以预料的是,碳化硅过滤器将显示与根据本文记载的实施例相似的结果。
样品制备
用于以下样品的过滤器基底由钛酸铝组成,其孔隙度为51%、平均孔尺寸为14μm~15μm,300cpsi和壁厚为13密耳。基底具有约2”×6”周长的尺寸。
对比例A
对比例催化剂具有以下组分:33.3g/ft3 Pt、16.7g/ft3Pd、0.5g/in3Siralox1.5/100(1.5%Si在Al2O3上)和0.1g/in3β沸石。沿着过滤器长度组成是相同的。
为了制备催化剂涂布浆料,借助始湿(incipient wetness)技术在行星混合器中中将四单乙醇胺氢氧化铂溶液浸渍于Siralox粉末上。然后使用相同的浸渍技术将硝酸钯施用至Pt/Siralox粉末上。然后将贵金属浸渍的粉末分散至水中以制备浆料。用连续研磨机研磨该浆料以将90%的颗粒度降低至小于4μm(D90<4μm)。在完成研磨前,将沸石加入浆料中。将所得浆料进一步用水稀释以获得19重量%固体。浆料的最终pH为4.1。
然后通过将基底浸入浆料中涂层浆料,基底入口向下、出口侧刚好高于浆料水平面(约1/4英寸)。从浆料中取出基底,然后用来自出口侧的气流吹气直到没有涂层浆料出现。然后将涂布的样品在110℃干燥2小时并且在450℃的空气中煅烧1小时。
实施例B
该实施例中使用D90<4μm的Ce/Zr复合材料(0.3g/in3)。使用Ce/Zr粉末而没有进一步减小颗粒度。用与实施例A中类似的方法涂层浆料。
实施例C
该样品中使用D90<13μm的铵形式的ZSM-5(0.3g/in3)。使用沸石粉末而没有进一步减小颗粒度。用与实施例A中类似的方法涂层浆料。
实施例D
该样品中使用研磨为D90<5μm的Siralox 1.5粉末(0.1g/in3)。用与实施例A中类似的方法涂层浆料。
实施例E
该样品中使用Siralox 1.5粉末(0.3g/in3)。在研磨前添加酒石酸以将粉末研磨为D90<6μm。从入口和出口侧两侧涂层浆料以使得总涂层负载量为0.3g/in3。
实施例F
使用喷射研磨的D90<7μm的氧化铝粉末。在连续研磨机中进一步将氧化铝粉末研磨为D90<5μm。从进口侧涂布浆料获得0.40g/in3的涂层。
图4显示实施例(样品)A~F的热膨胀系数(CTE)的图。这些测量在1000℃下完成。越低的CTE表示越坚固的催化烟灰过滤器。所有的研磨样品(实施例B~F)显示低于对比例A的CTE。已经观察到CTE小于15×10-7/℃的催化烟灰过滤器是坚固的。正在研究CTE为15×10-7~25×10-7/℃的坚固性。所有研磨样品的CTE为小于25×10-7/℃,多数低于15×10-7/℃。
实施例G~I
喷射研磨的D90<7μm的氧化铝粉末,进一步机械分级为3部分——精细粉末(实施例G)、中等粉末(实施例H)和粗糙粉末(实施例I)。图5中显示颗粒度分布(PSD)。实施例G的精细粉末,10%的颗粒具有小于约1.1μm的尺寸(90%>1.1μm)。实施例H的中等粉末,10%的颗粒具有小于约1.7μm的尺寸(90%>1.7μm)。实施例I的粗糙粉末,10%的颗粒具有小于约2.0μm的尺寸(或90%>2.0μm)。
分级粉末的各部分用作制备催化烟灰过滤器的氧化铝载体。将氧化铝粉末加入水中制备氧化铝浆料。将四单乙胺铂逐滴加入浆料中,然后将硝酸钯以相同方式加入浆料中。将浆料涂层在钛酸铝基底上。基底的孔隙度为约51%,平均颗粒度为约14~15μm,孔隙密度为约300cpsi,和壁厚为约13密耳。基底尺寸为2”×6”周长。涂布的过滤器在110℃干燥2小时,然后在450℃锻烧2小时。Pt和Pd的量等于23.3g/ft3 Pt和11.7g/ft3Pd。氧化铝的量为0.35g/in3。各涂布过滤器的涂层负载量相同。
从25°~1000℃测量各涂布过滤器的热膨胀系数(CTE)。在1000℃的CTE值概括在图6中。涂布“精细”、“中等”和“粗糙”氧化铝粉末的过滤器的CTE分别为约20.5、12.3和10.0。
对比例J~L
借助始湿技术在行星混合器中中将四单乙醇胺氢氧化铂溶液浸渍于Siralox粉末上。将乙酸(5重量%相对于粉末)加入粉末中。然后将贵金属浸渍的粉末分散至水中以制备浆料。用连续研磨机研磨该浆料以将90%的颗粒度降低至小于4μm(D90<4μm)。在完成研磨前,将Ce/Zr粉末加入浆料中。然后通过将过滤器基底浸入浆料中涂层浆料,基底入口向下、出口侧刚好高于浆料水平面(约1/4英寸)。从浆料中取出基底,然后用来自出口侧的气流吹气直到涂层浆料停止出现。然后将涂布的样品在110℃干燥2小时并且在450℃的空气中煅烧2小时。将三种基底涂布相同的浆料以获得以下催化剂组合物,5g/ft3、0.2g/in3Siralox,0.1g/in3Ce/Zr。三种基底的性能记载在表1中。
表1
实施例 | 基底 | 尺寸(mm) | CPSI | 壁厚(密耳) | 孔隙率(%) | 平均孔尺寸(μm) |
J | 钛酸铝 | 143.8×143.8×152.4 | 270 | 16 | 52 | 15 |
K | 堇青石类型1 | 143.8×143.8×152.4 | 250 | 15 | 50 | 20 |
L | 堇青石类型2 | 143.8×143.8×152.4 | 300 | 16 | 48 | 12 |
实施例M~O
干磨氧化铝粉末用于涂料。该氧化铝粉末具有以下颗粒度分布(PSD):90%的颗粒小于<5μm且90%的颗粒大于1.1μm。湿磨浆料(来自实施例J~L)和干磨氧化铝(本实施例)之间的PSD对比在图7中显示。
将氧化铝粉末加入水中制备氧化铝浆料。将四单乙胺铂逐滴加入浆料中,然后将硝酸钯以相同方式加入浆料中。将浆料涂层至表1中所示的各三个过滤器基底上。涂布的过滤器在110℃干燥2小时,然后在450℃锻烧2小时。金属和涂层负载量与用于参考样品中的相同。
图8显示参考样品(实施例J~L)和由具有更少精细颗粒的干磨氧化铝粉末制备的样品(实施例M~O)的CTE(在800℃测量)的对比。对各过滤器基底,通过使用具有更少精细颗粒的粉末显著降低了CTE。
实施例P~Q
用于样品P和Q的催化剂涂层包含相同量的贵金属(50g/ft3,Pt/Pd=2∶1)和基底金属组分(0.4g/in3载体,0.1g/in3β沸石)。将两种样品涂布在相同类型的过滤器基底上(SiC,50%孔隙度、平均孔尺寸=20μm,300cpsi,12密耳壁厚)。然而,通过不同方法制备涂层浆料。样品P通过与样品A相同的方法制备。样品Q通过与样品M相同的方法制备。
在流动反应器系统中用包含1000ppm的CO、基于C1的450ppm的烃类、100ppm的NO、10%的O2、7%的水、5%的CO2、其余为N2的进料测试催化烟灰过滤器(样品P和Q)。烃类组成是丙烯、甲苯和癸烷的等同份数,全部基于C1。用于测试的空间速度为35,000h-1。系统安装有CO、HC、CO2分析器以及FTIR分光光度计和质谱仪,其用来测定催化剂的转化效率。催化剂首先在90℃用进料饱和90秒,然后将温度以20℃/min斜线上升至300℃。连续监测和记录反应物和产物的浓度。CO和总烃类(THC)在各种时间下的转化率计算为进料中的浓度(未通过催化剂)与所得浓度(通过催化剂后)之间的相对差。测试前,将样品在装置中用流动空气和10%蒸汽在700℃下老化4小时,然后将样品在装置中在800℃下老化另外4小时。
图9显示了样品P和Q的催化性能(CO和HC点火曲线)的对比。与样品P的那些相比,用于样品Q的CO与HC两者均在低得多的温度点火(更活性)。样品Q上的CO的T50(定义为在50%转化率的温度)比样品P的低14℃,以及对HC T50的差值为36℃。根据一个或多个实施方案,当根据如上所述实施例P和Q的方法测试时,催化烟灰过滤器对一氧化碳显示低于约130℃的T50。在其它实施方案中,当根据实施例P和Q中相同方法测试时,催化烟灰过滤器对烃类显示低于约130℃的T50。在其它实施方案中,当在这些条件下测试时,催化烟灰过滤器对一氧化碳和烃类显示低于约130℃的T50。在其它实施方案中,当根据实施例P和Q的方法测试时,催化烟灰过滤器对烃类显示的T70(70%转化率)为低于约180℃、或低于约160℃、或低于约140℃或低于约130℃。
因此,虽然本发明已与其各种实施方案结合公开,应理解其它实施方案可以落在本发明的精神和范围内,如以下权利要求所限定。
贯穿本说明书的术语“一个实施方案”、“某些实施方案”、“一个或多个实施方案”或“实施方案”是指关于实施方案记载的特殊特征、结构、材料、或特性包括在本发明的至少一个实施方案中。因此,贯穿本说明书的许多地方出现的术语如“在一个或多个实施方案中”、“在某些实施方案中”、“在一个实施方案中”或“在实施方案中”不一定是指本发明的相同实施方案。此外,特殊的特征、结构、材料或特性可在一个或多个实施方案中以任何合适的方式结合。
尽管已经参考特殊实施方案描述本发明,可以理解的是这些实施方案仅仅是本发明的原理和应用的说明。对于本领域技术人员显而易见的是,可以对本发明的方法和装置进行各种改进和变化,而没有脱离本发明的精神和范围。因此,本发明意图包括在所附权利要求和它们的等同方式的范围内的改进和变化。
Claims (10)
1.一种催化烟灰过滤器,包括
壁流块料,其具有多个由纵向延伸壁形成的纵向延伸通道,纵向延伸壁划定所述通道的边界并限定所述通道,通道包括具有开放的入口端和封闭的出口端的入口通道,和具有封闭的入口端和开放的出口端的出口通道,壁流块料包含平均宽度小于0.4μm的微裂纹,和平均孔尺寸为10μm~25μm的孔;和
在壁流块料的壁内设置的涂层,所述涂层包括含有载体颗粒和至少一种贵金属的催化剂,其中至少90%的载体颗粒具有大于微裂纹的平均尺寸的颗粒度并且至少90%的载体颗粒具有小于壁流块料的孔的平均尺寸的颗粒度。
2.根据权利要求1的催化烟灰过滤器,其中至少90%的载体颗粒的颗粒度大于0.5μm。
3.根据权利要求1的催化烟灰过滤器,其中至少90%的载体颗粒的颗粒度大于1μm。
4.根据权利要求1的催化烟灰过滤器,其中至少60%的载体颗粒的颗粒度为1μm~5μm。
5.根据权利要求1的催化烟灰过滤器,其中所述载体颗粒选自铝化合物、锆化合物、铈化合物、沸石、硅化合物、基底金属氧化物及其组合组成的组。
6.根据权利要求1的催化烟灰过滤器,其中所述壁流块料包含孔隙率为40%~70%的钛酸铝。
7.根据权利要求1的催化烟灰过滤器,其中当在1000℃测量时,所述烟灰过滤器的热膨胀系数小于25×10-7/℃。
8.根据权利要求7的催化烟灰过滤器,其中当在800℃测量时,所述烟灰过滤器的热膨胀系数小于5×10-7/℃。
9.根据权利要求1的催化烟灰过滤器,其中所述过滤器对烃类显示的T70温度低于180℃,其中过滤器用流动空气和10%蒸汽在700℃下老化4小时,然后在800℃下老化4小时,并且在流动反应器系统中用包含1000ppm的CO、基于C1的450ppm的烃类、100ppm的NO、10%的O2、7%的水、5%的CO2、其余为N2的进料测试,烃类组成是丙烯、甲苯和癸烷的基于C1的等同份数,测试通过用进料气体在90℃饱和过滤器90秒,然后将温度以20℃/min斜线上升至300℃而进行。
10.一种制备催化剂涂布的壁流块料的方法,所述催化剂涂布的壁流块料包含平均宽度小于0.4μm的微裂纹和平均孔尺寸为10μm~25μm的孔,该方法包括
提供壁流块料,其具有多个由纵向延伸壁形成的纵向延伸通道,纵向延伸壁划定所述通道的边界并限定所述通道,通道包括具有开放的入口端和封闭的出口端的入口通道,和具有封闭的入口端和开放的出口端的出口通道,以及用包含可热分解的催化材料和固体颗粒的含水浆料的形式的涂层涂布壁流块料,至少90%的颗粒具有大于微裂纹的平均尺寸的颗粒度,且至少90%的颗粒具有小于孔的平均尺寸的颗粒度;以及
将涂布的壁流块料加热至足够干燥涂层的温度。
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US11/959,090 US8114354B2 (en) | 2007-12-18 | 2007-12-18 | Catalyzed soot filter manufacture and systems |
US11/959,090 | 2007-12-18 | ||
US12/336,070 | 2008-12-16 | ||
US12/336,070 US8038956B2 (en) | 2007-12-18 | 2008-12-16 | Catalyzed soot filter manufacture and systems |
PCT/US2008/087245 WO2009079590A1 (en) | 2007-12-18 | 2008-12-17 | Catalyzed soot filter manufacture and systems |
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CN2008801218020A Active CN101970088B (zh) | 2007-12-18 | 2008-12-17 | 催化烟灰过滤器的制造和系统 |
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US (2) | US8114354B2 (zh) |
EP (1) | EP2240259A1 (zh) |
JP (3) | JP2011506095A (zh) |
KR (1) | KR101629034B1 (zh) |
CN (1) | CN101970088B (zh) |
CA (1) | CA2708235C (zh) |
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JP2017121624A (ja) | 2017-07-13 |
CA2708235A1 (en) | 2009-06-25 |
CN101970088A (zh) | 2011-02-09 |
US20090155135A1 (en) | 2009-06-18 |
BRPI0820724A2 (pt) | 2015-06-16 |
CA2708235C (en) | 2016-06-21 |
ZA201005017B (en) | 2011-09-28 |
KR20100106497A (ko) | 2010-10-01 |
KR101629034B1 (ko) | 2016-06-09 |
MY152756A (en) | 2014-11-28 |
JP6379166B2 (ja) | 2018-08-22 |
WO2009079590A1 (en) | 2009-06-25 |
EP2240259A1 (en) | 2010-10-20 |
US8114354B2 (en) | 2012-02-14 |
US20090155134A1 (en) | 2009-06-18 |
US8038956B2 (en) | 2011-10-18 |
JP2011506095A (ja) | 2011-03-03 |
JP2015157285A (ja) | 2015-09-03 |
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