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CN117098591A - 用于从汽油内燃机的废气中减排氨的催化剂 - Google Patents

用于从汽油内燃机的废气中减排氨的催化剂 Download PDF

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Publication number
CN117098591A
CN117098591A CN202280025338.5A CN202280025338A CN117098591A CN 117098591 A CN117098591 A CN 117098591A CN 202280025338 A CN202280025338 A CN 202280025338A CN 117098591 A CN117098591 A CN 117098591A
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catalyst
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material region
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Inventor
M·科伦坡
C·布劳恩
M·施密特
M·塞勒
P·塞尔韦
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Umicore AG and Co KG
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Umicore AG and Co KG
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Publication of CN117098591A publication Critical patent/CN117098591A/zh
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Abstract

本发明涉及一种催化剂，该催化剂包括具有在第一端面和第二端面之间延伸的长度L的载体主体以及布置在载体主体上的不同组成的材料区A、材料区B和材料区C，其中材料区A包括铑和/或镍和/或铈；材料区B包含铂；并且材料区C包含能够储存氨并催化NOx的选择性催化还原的沸石。

Description

用于从汽油内燃机的废气中减排氨的催化剂
本发明涉及一种用于从汽油内燃机的废气中减排氨的催化剂，该催化剂包括若干材料区。
在燃烧式发动机领域中众所周知，燃料燃烧是不完全的，并产生污染物排放，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。就客车这样的移动源来说，主要措施能够实现污染物排放减少。改进燃料-空气混合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。在λ＝1+/-0.005附近，即空燃比等于14.56的情况下，TWC的使用最佳。高于这些值，废气被称为稀薄，并且CO和HC被催化氧化成二氧化碳和水。低于该值，废气称作富集，并且NOx主要使用例如CO作为还原剂而被还原成氮气N2。
在λ＝1时实现HC、CO和NOx的最佳转化率。然而，汽油发动机在振荡条件下运行，即处于略微稀薄和略微富集的条件之间。在纯富集的条件下，碳氢化合物的转化率迅速下降。为了拓宽TWC的最佳运行，在TWC的配方中包括了呈Ce混合氧化物形式的储氧材料(OSM)。
在某些操作条件下，氨可在TWC催化剂上形成，导致氨存在于废气料流中。考虑到其毒性作用，这是不期望的，因此在废气法规中氨排放越来越受到限制。
为了避免氨排放，已经开发了所谓的氨逃逸催化剂(ASC)并且主要用于现代柴油发动机的废气中。ASC催化剂通常含有铂族金属(PGM)组分，特别是铂，以在尽可能低的温度下进行氨的氧化。然而，PGM基材料不仅将氨氧化成氮气，而且还可以形成氮氧化物，特别是N2O、NO和NO2。为了改进氨氧化组分的选择性，通常将其与SCR催化剂组合，该SCR催化剂用于再还原所形成的氮氧化物。可使用的SCR催化剂例如是不同空间布局的沸石基或钒基。在分层布局的情况下，SCR层通常覆盖含PGM的层。
这种概念不能简单地引申到汽油发动机的废气上，因为氨不能在由汽油发动机排出的富集废气中被氧化。因此，在将ASC催化剂应用于汽油发动机的废气的情况下需要不同的工作模式。在富集阶段操作期间，SCR层充当缓冲区，储存由上游TWC产生的氨。在稀薄阶段操作期间，当氧存在于废气料流中时，氨可被PGM层氧化。
此种操作模式具有以下限制。首先，可储存的氨的量受限于SCR层的氨储存容量。一旦达到容量，将发生氨排放。该问题在催化剂老化后可能甚至更严重，老化通常导致氨储存容量的损失。第二，在给定温度下储存在SCR层上的氨可以在温度升高之后的任何时间解吸。若在富集操作期间时发生这样的温度上升，则氨不会被ASC催化剂转化，从而导致氨排放。
因此，需要一种解决方案来克服这些限制并且进一步降低在汽油发动机的废气中氨排放的可能性。
GB1453456A公开了将氨分解成氮气和氢气的催化剂。此类催化剂包括NiO和含NiO的材料。据说含有大量NiO(约超过50摩尔％)的催化剂对氨的分解表现出显著的催化作用。
EP0723805A2描述了一种方法，该方法包括在还原气氛中(例如经由三元催化剂)将NOx组分转化为氨，并且当催化剂的温度在预先确定的温度范围内时在氧化气氛中经由NH3分解催化剂将氨分解。
现已发现下文描述和定义的催化剂解决了上述问题。
本发明涉及一种催化剂，其包括具有在第一端面和第二端面之间延伸的长度L的载体主体以及布置在所述载体主体上的不同组成的材料区A、材料区B和材料区C，其中
-材料区A包含铑和/或镍和/或铈，
-材料区B包含铂，并且
-材料区C包含能够储存氨并催化NOx的选择性催化还原的沸石。
在材料区A包含铑的情况下，铑优选以铑金属的形式存在。在材料区A包含镍的情况下，镍优选以氧化镍的形式存在，特别是以NiO的形式存在。在材料区A包含铈的情况下，铈优选以二氧化铈的形式存在，特别是CeO2。
在材料区包含铑的情况下，基于载体主体的体积并以铑金属计算，铑通常以0.01g/l至1g/l的量存在。
在材料区包含镍的情况下，基于载体主体的体积并以NiO计算，镍通常以1g/l至100g/l的量存在。
在材料区包含铈的情况下，基于载体主体的体积并以CeO2计算，铈通常以1g/l至100g/l的量存在。
在材料区A包含铑和镍的情况下，以铑金属和NiO计算，铑和镍的重量比优选为1:1000至1:1，更优选为1:130至1:70。
在材料区A包含铑和铈的情况下，以铑金属和CeO2计算，铑和铈的重量比优选为1:1000至1:1，更优选为1:130至1:70。
在材料区A包含镍和铈的情况下，以NiO和CeO2计算，镍和铈的重量比优选为1:100至100:1，更优选为1:3至3:1。
通常，材料区A包含负载在一种或多种载体氧化物A上的铑和/或镍和/或铈。
合适的载体氧化物A有利地为高熔点的，即其熔点足够高于在根据本发明的催化剂的预期操作期间出现的温度。其还有利地具有高表面积并优选具有50m2/g至200m2/g的BET表面(根据DIN 66132测定)。
载体氧化物A特别是选自由以下项组成的组：氧化铝、掺杂的氧化铝、氧化硅、二氧化钛、掺杂的氧化钛、氧化锆以及它们中的一种或多种的混合氧化物以及沸石。如果材料区A包含铑和/或镍，则载体氧化物A也可以是二氧化铈。
掺杂的氧化铝例如是用氧化硅、氧化锆和/或氧化钛掺杂的氧化铝以及镧掺杂的氧化铝。在后者中，各自以La2O3计算并相对于稳定化的氧化铝的重量计，镧以1重量％至10重量％，优选3重量％至6重量％的量使用。
可用作载体氧化物A的沸石例如为结构类型ABW、AEI、AFX、BEA、CHA、DDR、ERI、ESV、FAU、FER、KFI、LEV、LTA、MER MFI、MWW、SOD或STT的沸石，并且优选不与铜和/或铁交换。
优选地，载体氧化物A是氧化铝。
材料区B包含铂，其优选以铂金属的形式存在。
基于载体主体的体积并以铂金属计算，材料区B通常包含0.017g/l至0.18g/l的量的铂。
通常，材料区B包含负载在载体氧化物B上的铂。
合适的载体氧化物B有利地为高熔点的，即其熔点足够高于在根据本发明的催化剂的预期操作期间出现的温度。其还有利地具有高表面积并优选具有50m2/g至200m2/g的BET表面(根据DIN 66132测定)。
特别地，载体氧化物B选自由以下项组成的组：氧化铝、掺杂的氧化铝、氧化硅、二氧化钛、掺杂的氧化钛、氧化铈、氧化锆以及它们中的一种或多种的混合氧化物以及沸石。
掺杂的氧化铝例如是用氧化硅、氧化锆和/或氧化钛掺杂的氧化铝以及镧掺杂的氧化铝。在后者中，各自以La2O3计算并相对于稳定化的氧化铝的重量计，镧以1重量％至10重量％，优选3重量％至6重量％的量使用。
可用作载体氧化物B的沸石例如为结构类型ABW、AEI、AFX、BEA、CHA、DDR、ERI、ESV、FAU、FER、KFI、LEV、LTA、MER MFI、MWW、SOD或STT的沸石，并且优选不与铜和/或铁交换。
优选地，载体氧化物B是氧化铝。
优选地，材料区B包含负载在氧化铝上的铂。
沸石是二维或三维结构，其最小结构可以被认为是SiO4和AlO4四面体。这些四面体聚在一起形成更大结构，其中两个四面体每次经由共用的氧原子连接。由此可以形成不同尺寸的环，例如四个、六个或甚至九个四面体配位的硅或铝原子的环。沸石的不同类型通常经由最大的环尺寸来定义，因为该尺寸决定哪些客体分子可进入沸石结构以及哪些客体分子不能进入沸石结构。通常区分最大环尺寸为12的大孔沸石、最大环尺寸为10的中孔沸石和最大环尺寸为8的小孔沸石。
此外，沸石由国际沸石协会结构委员会(Structural Commission of theInternational Zeolite Association)分组成以三字母代码提供的结构类型。参见例如Atlas of Zeolite Framework Types,Elsevier,5th edition,2001(《沸石框架类型图集》，Elsevier，第5版，2001年)。
能够储存氨并催化NOx的选择性催化还原的材料区C的沸石可以是大孔、中孔或小孔沸石，并与铜或铁交换。合适沸石的示例属于结构类型ABW、AEI、AFX、BEA、CHA、DDR、ERI、ESV、FAU、FER、KFI、LEV、LTA、MER MFI、MWW、SOD或STT。
优选地，材料区C的沸石是铜交换的并且特别属于结构类型AEI、AFX、CHA或LEV，或者是铁交换的并且特别属于结构类型BEA。
更优选地，材料区C的沸石是Cu-AEI、Cu-CHA或Fe-BEA。
材料区C的沸石优选地具有2至100，更优选5至50，并且最优选10至40的SAR(二氧化硅/氧化铝比率)值。
在本发明的上下文中，术语沸石还包括分子筛，其有时也称为“类沸石”化合物。属于上述结构类型之一的分子筛为优选的。示例包括术语名称为SAPO的磷酸硅铝沸石和术语名称为AlPO的磷酸铝沸石。
任选地，本发明催化剂的载体主体包括含有沸石的材料区D，该沸石能够储存氨并催化NOx的选择性催化还原。
材料区D可以与材料区C相同，这意味着包含相同量的相同组分。材料区D也可以不同于材料区C。在后一种情况下，它可以例如包含相同的组分但以不同的量包含，或者它可以包含完全或部分不同的组分。
根据本发明的催化剂包括载体主体。这可为流通式基材或壁流式过滤器。
壁流式过滤器是负载主体，其包括长度为L的通道，该通道在壁流式过滤器的第一端和第二端之间平行地延伸，它们在第一端或第二端处交替地密封，并且由多孔壁分开。具体地，流通式基材与壁流式过滤器的不同之处在于长度为L的通道在其两端是敞开的。
在未涂覆状态下，壁流式过滤器具有例如30％至80％、具体地50％至75％的孔隙率。在未涂覆状态下，它们的平均孔径例如为5微米至30微米。
一般来讲，壁流式过滤器的孔是所谓的开放孔，即它们与通道连接。此外，孔通常彼此互连。这使得一方面能够容易地涂覆内孔表面，并且另一方面使废气容易通过壁流式过滤器的多孔壁。
流通式基材是本领域技术人员已知的，壁流式过滤器也是如此，并且均可商购获得。它们由例如碳化硅、钛酸铝或堇青石组成。
通常，材料区A、材料区B、材料区C和材料区D(如果存在的话)以涂层的形式存在于载体主体上，换言之，在载体主体上形成载体涂料层或载体涂料区。它们可以各种方式布置在载体主体上。
在第一实施方案中，
-材料区A从载体主体的第一端面开始在长度L的10％至90％上延伸，
-材料区B从载体主体的第二端面开始在长度L的10％至90％上延伸并且
-材料区C从载体主体的第二端面开始在长度L的10％至90％上延伸，
其中L＝LA+LB，其中LA为材料区A的长度并且LB为材料区B的长度，并且
其中材料区C位于材料区B的顶部。
在优选的第一实施方案中，材料区A、材料区B和材料区C都在长度L的40％至60％的长度上延伸。
在更优选的第一实施方案中，材料区A、材料区B和材料区C都在长度L的50％上延伸。
在第二实施方案中，
-材料区A从载体主体的第一端面开始在长度L的10％至90％上延伸，
-材料区B从载体主体的第二端面开始在长度L的10％至90％上延伸，
-材料区C从载体的第二端面开始在长度L的10％至90％上延伸，
并且
-材料区D从载体的第一端面开始在长度L的10％至90％上延伸，
其中L＝LA+LB＝LC+LD，其中LA是材料区A的长度，LB是材料区B的长度，LC是材料区C的长度，并且LD是材料区D的长度，并且
其中材料区C位于材料区B的顶部，并且材料区D位于材料区A的顶部。
在优选的第二实施方案中，材料区A、材料区B、材料区C和材料区D都在长度L的40％至60％的长度上延伸。
在更优选的第二实施方案中，材料区A、材料区B、材料区C和材料区D都在长度L的50％上延伸。
在甚至更优选的第二实施方案中，材料区A、材料区B、材料区C和材料区D都在长度L的50％上延伸，并且材料区C和材料区D是相同的。这意味着材料区C和材料区D在材料区A和材料区B的顶部形成均匀的层。
根据本发明的催化剂可通过以本身已知的方式使用涂料悬浮液(所谓的载体涂料)涂覆适宜的载体主体来制备。
该悬浮液通过技术人员已知的方法获得，并且然后通过标准涂覆方法中的一种研磨并施用于载体主体。在每个涂覆步骤后，经涂覆的部分在热空气流中干燥并在一些情况下煅烧。
根据本发明的催化剂适用于净化汽油发动机的废气，特别是它们适用于消除由上游三元催化剂形成的氨。材料区A、材料区B和材料区C具有不同的功能。在不存在氧的情况下，即在富集操作条件下，材料区A负责氨到氮的催化分解。在氧存在下，即在稀薄操作条件下，材料区B负责氨的氧化。最后，材料区C和材料区D(如果存在的话)负责氨的储存和释放。
因此，本发明还涉及一种从汽油废气中消除氨的方法，其特征在于，穿过如上所述和定义的催化剂引导该汽油废气。在该方法的一个实施方案中，汽油废气在第一端面流入载体主体中并在第二端面流出载体主体。在该方法的另一实施方案中，汽油废气在第二端面流入载体主体中并在第一端面流出载体主体。
根据本发明的催化剂特别地用作包括三元催化剂的废气净化系统的组成部分。在这种体系中，本发明的催化剂被布置成使得废气首先流过三元催化剂，随后流过根据本发明的催化剂。
除了三元催化剂和本发明的催化剂之外，废气净化系统可以包括所谓的汽油微粒过滤器(GPF)，其能够减少或消除汽油发动机的废气中所含的颗粒排放。
三元催化剂和汽油颗粒过滤器是本领域技术人员已知的并且广泛描述于文献中，包括相关教科书。
图1示出了本发明的催化剂，其中材料区A、材料区B和材料区C都在长度L的50％上延伸，并且其中材料区A从载体主体的第一端面开始，并且材料区B和材料区C从载体主体的第二端面开始。
图2示出了本发明的催化剂，其基于图1中所示的催化剂，但其另外包括材料区D，该材料区D从第一端面开始在长度L的50％上延伸并且位于材料区A上。

Claims (14)

1.一种催化剂，所述催化剂包括具有在第一端面和第二端面之间延伸的长度L的载体主体以及布置在所述载体主体上的不同组成的材料区A、材料区B和材料区C，其中
-材料区A包含铑和/或镍和/或铈，
-材料区B包含铂，并且
-材料区C包含能够储存氨并催化NOx的选择性催化还原的沸石。
2.根据权利要求1所述的催化剂，其特征在于，基于所述载体主体的体积并以铑金属计算，材料区A包含0.01g/l至1g/l的量的铑。
3.根据权利要求1和/或2所述的催化剂，其特征在于，基于所述载体主体的体积并以NiO计算，材料区A包含1g/l至100g/l的量的镍。
4.根据权利要求1至3中的一项或多项所述的催化剂，其特征在于，基于所述载体主体的体积并以CeO2计算，所述材料区A包含1g/l至100g/l的量的铈。
5.根据权利要求1至4中的一项或多项所述的催化剂，其特征在于，材料区B包含负载在氧化铝上的铂。
6.根据权利要求1至5中的一项或多项所述的催化剂，其特征在于，材料区C包含Cu-AEI、Cu-CHA或Fe-BEA。
7.根据权利要求1至6中的一项或多项所述的催化剂，其特征在于，所述催化剂包括材料区D，所述材料区D包含能够储存氨并且能够催化NOx的选择性催化还原的沸石。
8.根据权利要求7所述的催化剂，其特征在于，材料区C和材料区D含有相同量的相同组分。
9.根据权利要求1至8中的一项或多项所述的催化剂，其特征在于，如果存在材料区D的话，所述材料区A、材料区B、材料区C和材料区D以涂层的形式存在于所述载体主体上。
10.根据权利要求9所述的催化剂，其特征在于，
-材料区A从所述载体主体的所述第一端面开始在长度L的10％至90％上延伸，
-材料区B从所述载体主体的所述第二端面开始在长度L的10％至90％上延伸，并且
-材料区C从所述载体主体的所述第二端面开始在长度L的10％至90％上延伸，
其中L＝LA+LB，其中LA为材料区A的长度并且LB为材料区B的长度，并且
其中材料区C位于材料区B的顶部。
11.根据权利要求9所述的催化剂，其特征在于，
-材料区A从所述载体主体的所述第一端面开始在长度L的10％至90％上延伸，
-材料区B从所述载体主体的所述第二端面开始在长度L的10％至90％上延伸，
-材料区C从所述载体主体的所述第二端面开始在长度L的10％至90％上延伸，并且
-材料区D从所述载体主体的所述第一端面开始在长度L的10％至90％上延伸，
其中L＝LA+LB＝LC+LD，其中LA是材料区A的长度，LB是材料区B的长度，LC是材料区C的长度，并且LD是材料区D的长度，并且其中材料区C位于材料区B的顶部，并且材料区D位于材料区A的顶部。
12.根据权利要求11所述的催化剂，其特征在于，材料区A、材料区B、材料区C和材料区D都在长度L的50％上延伸，并且材料区C和材料区D是相同的。
13.一种从汽油废气中消除氨的方法，其特征在于，穿过根据权利要求1至12中的一项或多项所述的催化剂引导所述汽油废气。
14.一种废气净化系统，所述净化系统包括三元催化剂和根据权利要求1至12中的一项或多项所述的催化剂。
CN202280025338.5A 2021-03-30 2022-03-29 用于从汽油内燃机的废气中减排氨的催化剂 Pending CN117098591A (zh)

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