CN1082662A - 催化转化反应器 - Google Patents

催化转化反应器 Download PDF

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CN1082662A
CN1082662A CN93103455A CN93103455A CN1082662A CN 1082662 A CN1082662 A CN 1082662A CN 93103455 A CN93103455 A CN 93103455A CN 93103455 A CN93103455 A CN 93103455A CN 1082662 A CN1082662 A CN 1082662A
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container
chamber
secondary air
downstream
catalyst
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A·布拉金
Y·布思拉夫
V·卡恩尔
N·莫瑟夫
R·蒙塔诺
E·苏思多罗维奇
K·索尔瑟夫
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Blue Planet Technologies Co LP
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Abstract

一种催化剂容器，包括在上游端的一个进口，位 于管道下游的多个催化室，其中至少两个室被其上带 有一个或多个孔的一平板连接，以允许气流从第一室 向第二室流动，并且其中在室的至少一个表面是适于 沉积从下组中选出的一种金属：该组包括铂、铑和铼， 以及一在容器下游端的出口。

Description

本发明涉及催化转化反应器，更具体的说涉及装有用于转化汽车排气的催化剂的反应器。
在同时燃烧从汽车发动机或类似设备排放的一氧化碳和未反应的碳氢化合物的氧化反应和氮氧化物（NOx）的还原反应的反应中，长期以来一直需要使用催化剂。催化剂的作用，特别是在汽车排气控制中三用催化剂（three-way  catalysts）在本领域中进行了广泛地研究。例如：Taylor的“汽车催化转化器”（见《Catalysis，Science  and  Technology，PP119-67，Anderson等，出版.1984）描述了排气控制技术、三用催化剂的组成和催化剂载体。
用于转化汽车排气的传统系统采用予制载体的催化剂，典型的为一种固体层状的催化剂材料，例如放置于汽车排气部分的蜂窝状的陶瓷结构。当排气通过该固体层时，存在于层状结构上的催化金属帮助CO、NOx和未燃烧碳氢化合物转化成CO2、N2和H2O。然而，在发动机排气部分的固体层状型催化转化器最终会因耗尽需要拆除和更换。此外，蜂窝之类的载体结构复杂且比较贵。依该技术界所述，能执行三用催化作用的体系包括那些带载体的铑和铂，而诸如铑之类的贵金属为优选的用于反应的催化剂：
Pi是CO和未燃烧碳氢化合物类氧化的优选催化剂。
贵金属价格高，货源有限，特别是铑。由于目前三用催化剂使用的铂和铑超过了Rh/Pi的矿藏比率而使情况更为严重。因此减少贵金属的使用是三用催化剂的一个问题。因而必须开发排气控制的其它方法。
因此，在汽车的排气系统中，需要其它的催化转化反应器，它可以转化汽车排气而不使用传统的其它的不可再生的含固体催化材料的载体。否则就需要具有高转化效率的其它的含金属催化剂的催化转化反应器，以便于减少所需要的催化剂的供给。
依上所述，本发明的一个目的是提供一种可转化汽车发动机排气的催化转化反应器。
本发明的再一个目的是提供一种可转化汽车排气的催化剂不需要在发动机的排气部分设置一种附加的不可再生的固体催化载体系统。
本发明的这些和其它的目的可由一种催化转化反应器实现，它包括：在上游端的一个进口，位于管道下游的多个催化室，其中至少两个由带有一个或多个小孔的平板连结，以允许气流从第一室进到第二室，并且在其中室的至少一个表面用来沉积由铂、铑和铼组成的组中选出的一种金属，以及在其下游端的一个出口。
图1是本发明的一种催化转化反应器的截面侧视图。
图2是用于本发明的催化转化反应器中的一种平板的截面视图。
本发明的催化转化反应器包括一个催化转化反应器，该反应器包括一个在上游端的进口，位于管道下游端的多个催化转化反应室，其中至少两个室由带有一个或多个小孔的平板连结，以允许气流从第一室流到第二室，并且在其中室的至少一个表面用来沉积由铂、铑和铼组成的组中选出的一种金属，以及在其下游端的一个出口。这种催化转化反应器在下述催化系统中是很有用的，这类催化系统包括一种液体金属催化剂源，往燃烧系统中添加金属催化剂的装置，该催化转化反应器收集金属催化剂，并且是转化原物料例如汽车排气至最终生成物的一个区域。
催化剂收集器位于燃烧室的下游。收集器收容催化剂，并且作为一个反应器，将汽车排气转化成CO2，N2和H2O。催化剂收集器有一能保持住催化剂并使足量催化剂可用于与流过收集器的汽车排气反应。
优选使收集器是一种消音器或一种象消音器的系统，他有一系列的盘和/或挡板和/或一个填充床，其中包含有填充床的是特别优选的。消音器的表面允许催化剂保持在收集器内，以将经过收集器的排气充分转化。优选使消音器表面制成能从催化剂溶液中保留金属的一种固体材料的结构，或是使消音器表面含有可以保留金属的裂缝或孔隙。适宜的消音器表面材料可以包括钢、铁、陶瓷和热固性聚合物，特别优选低碳钢。低碳钢是指含碳量低于0.5%（重量）的钢。
在一特别优选实施例中，消音器还包括一种可留住金属催化剂的填料。已经发现，铁和铁的化合物以及钢，特别是低碳钢，呈屑状时非常有利于本发明的实际应用。其它适用的填料包括陶瓷、热固性聚合物，和可以留住金属催化剂的其他多孔材料。在使用低碳钢屑时，最好酸洗后再填入消音器中。酸洗优选用1M的HCl溶液。当金属催化剂带入消音器时，催化剂沉积在钢屑的孔隙中。从燃烧室来的排气经过消音器时即可以与催化剂接触，并被转化成N2，CO2和H2O。CO和未燃烧碳氢化合物被氧化，而NOx在金属所在区域被还原。在转化后，生成物被解吸，使得该位置可再次用于转化。催化反应优选一种三用催化反应：氧化CO，氧化未燃烧的碳氧化合物和还原NOx。也可任选地，使用一种其它的氧化催化剂以提高由燃烧室排出的CO和未燃烧碳氢化合物的转化率。
在另一实施例中，可以加入二次空气到催化剂收集器中以促进CO和未燃烧碳氢化合物的氧化，不用或者仍然用任选的氧化催化剂。在使用二次空气时，二次空气加入量约为流过消音器气流体积的1%到15%。优选用约2%到4%的二次空气。
参见附图1，它示出了本发明的一种催化转化反应器。该催化转化反应器带有一进气管10，最好使其上游端12与一汽车发动机的燃烧系统相连结。管10在其下游端与收集器14相连结。收集器包括三个互相分开的室16、18、20。第一室16最好装有低碳钢屑，并且实质上是NOx还原的区域。第二室18是用作从二次空气进气管22进入的二次空气与经过第一室的排气的混合增强器。第三室20装有低碳钢屑，实质上是氧化CO和未燃烧碳氢化合物的区域。从进气管22加入的二次空气是用作促进在第三室20的氧化反应。
催化转化反应器14的三个室被带有孔的板24、26分隔。带孔的板24、26优选用与第一、第二和第三各室16、18、20中的填料相同的材料制造。参看图2，它示出了一种适用于分隔催化转化反应器14各室的一种板。如图2所示，这种板带有许多个小孔28。这些孔可以随意地设制在该板上，或采取任何要求的图形。这些孔可以是任何合适的形状，优选圆形的或椭圆形的孔。孔的数量和尺寸可以变动，只要在板上全部孔的面积足以允许一适当的体积流速到邻近的下游室去。全部孔的面积必须足够小，以保持住其邻室内的填料，同时对该系统提供低阻力和背压。
再参看图1，进气管22优选用钢制造，并且联接到诸如由皮带驱动的空气压缩机之类的气源上。最好让进气管22用来输送高达进入第三室的体积流量的15%的足量空气。特别优选让进气管22提供约2%至4%的进入第三室20的体积流量。二次空气进口22对收集器14提供过量空气以帮助氧化反应，特别是帮助一氧化碳氧化成CO2。
优选使各室16、18和20装有一种填料，例如呈屑状的低碳钢。对于典型的汽车排放系统来说，使用低碳钢作为填料时，最好让各室的填料为约0.1至0.5磅。优选让各室所装有的低碳钢填料为约0.2至1磅。
优选的填料制备方法包括：（a）用一种有机溶剂，例如乙醇，清洗该填料，（b）用水或其他适合的清洗剂洗去有机溶剂，然后（c）用一种碱性化合物冲洗，（d）用水或其他合适的清洗剂洗涤，然后（e）酸洗填料，并且（f）用水或其他合适的清洗剂洗涤。已经发现用盐酸洗可获得非常有效的填料。特别优选1M的盐酸溶液用于酸洗工序。
优选让填料以内骨架结构置于各室16、18、20中以使填料在各室16、18、20中分布令人满意。在各室没有内骨架结构的地方，填料的沉积会在该室顶部引起气流穿透，该处就会发生不充分的排气转化作用。
该骨架结构最好由多个水平穿过各室的格网组成，相互之间呈平行地分布。填料则被放置在格网上，以供16、18、20各室的基本上的整个区域都进行废气转化。填料优选有最佳密度，以便必须提供要求的废气转化率，又不使通过室的气流产生过大的背压。低密度填料室会产生不充分的废气转化作用，而高密度填料室会不必要地增加流过该室的气流背压。16、18、20各室的填料密度优选为约0.5至1501bS/ft3。已经发现填料密度约为10至151bS/ft3特别合适。
位于第三室20下游的是一个氧化催化剂结构30。该氧化结构30优选含氧化催化剂例如铁、钢、铜或它们的化合物，例如铁或铜的氧化物，特别优选铜的氧化物。结构30的氧化催化剂最好制成薄片状，卷紧后置入结构30内。一排气管32位于氧化催化结构30的下游。排气管32通向本系统的出口处，例如通向大气。
在运行中，容器14是用作催化剂收集，并且是反应的场所。两件共悬未决的美国申请07/841356和07/841357（都在1992年2月25日被受理）更充分地描述了一种可用作金属催化剂源的催化剂溶液，和可以加入到本发明的催化转化反应器中去的一种催化系统。这两篇申请的说明书本文借用作参考。优选让催化剂来源是一种液体催化剂溶液，后者在一种合适的溶剂中含有一种或多种金属化合物。对本发明有用的金属包括中间过渡族金属，特别是ⅦA族的金属，例如铼（Re），和末尾过渡金属，例如ⅧA族金属，包括铂和铑。这些金属在溶液中呈化合物态，例如氯化物、羰基化合物、高铼酸盐和氧化物。优选的金属化合物的溶剂包括二醇衍生物类，特别是二甘醇的衍生物，例如二甘醇二甲醚[CH3O（CH2）2]2O，三甘醇二甲醚和四甘醇二甲醚。其他优选的溶剂包括烷基毗咯烷酮类，例如N-甲基吡咯烷酮，和烷氧基乙基醚，例如双-[2-（2-甲氧基-乙氧基）乙基]醚。二甘醇二甲醚是特别优选的溶剂，在最优选的实施例中，溶液为在二甘醇二甲醚中含有H2PtCl6·6H2O、LiReO4和RhCl3·4H2O。
溶液用泵或喷雾的方法引入催化系统内，喷雾的方法是引入溶液的小液滴。在溶液中的金属催化剂通过系统，最好通过汽车发动机的进气管经过燃烧室而到进气管12。金属催化剂从管道12进入到容器14内，在那里沉积到表面上，例如16、18、20各室的内壁上，或在这些室内放置的填料上。这样，金属催化剂就作为反应的场所，让燃烧室来的排气经进气管12进入容器14进行反应。
虽然没有希望被理论所发现，但是可以认为：金属催化剂化学吸附在表面上，并且分散在表面上，从而可以获得很大的贵重的金属表面积用于反应。可以相信本发明的系统比传统的催化转化器可获得更多的金属催化剂原子用于反应。
一旦催化剂被化学吸附到容器14的表面上，可以认为，一种传统的排气三用催化剂就出现了。这就是未燃烧的碳氢化合物被氧化、CO被氧化，NOx被还原成H2O，CO2和N2。未燃烧的碳氢化合物中，据信链烯烃的、其他不饱和烃、以及环烃，最易被氧化，饱和烃类，特别是甲烷，较比不易地被氧化。可以认为，相对于存在于排气中的CO来说，未燃烧的碳氢化合物一般易于被氧化。在氧化反应和还原反应进行之后，生成物H2O、CO2和N2被解吸，腾出的反应场所再用于催化反应。在容器14中催化剂可以用添加催化加料溶液到该系统中的方法周期性地补充。
可以认为这种三用催化剂大体上存在于从管12的进口端到氧化30的出口端的各处。然而已经发现按比例来说较大量的还原反应发生在靠近容器14进口的部位，而较大量的氧化反应发生在靠近容器14的出口部位。这是因为，第一室16有整个还原反应过程中较大的场所，而第三室20有催化转化反应器14中整个氧化反应过程较大的场所。
在第一室16中，被认为占主导地位的化学反应是：
这里HC代表未燃烧的碳氢化合物。
在第三室20中，被认为占主导地位的化学反应是：
当排出物通过容器14的出口时，它们被输送通过氧化催化结构30。氧化结构30的作用是把通过催化转化反应器14的未反应的CO和未燃烧的碳氢化合物进行氧化以增加该系统的氧化效果。排出物此时基本上没有CO、NOx和未燃烧的碳氢化合物通过排气管32排出，例如排到大气中。
使用本发明的催化系统，汽车的发动机允许在较恶劣的工况下运行，因而提高了燃料的经济性。传统的汽车发动机为适于有效地转化排气以满足目前美国污染程度的要求（要求转化76%的NOx，94%的CO和94%的未燃烧碳氢化合物）必须以约0.9至1.03的空气值运行（1.0空气值相当于化学计算量的空气燃料比，为14.7∶1以重量计）。使用本发明的催化系统，发动机能够以高于1.10的空气值下运行，并仍满足污染程度的要求。

Claims (10)

1、一种催化剂容器，包括上游端的一进口，位于导管下游的多个催化室，其中至少两个室由其上带有一个或多个小孔的平板连结，以允许气流从第一室流到第二室，并且其中在室内的至少一个表面是适于沉积从含有铂、铑和铼的组中选择的一种金属，以及一种在其下游端的出口。
2、依据权利要求1的一种容器，其中，适于金属沉积的表面包括一种在至少一个室内的填料。
3、依据权利要求2的一种容器，其中所述的填料是从包括钢、铁、陶瓷和热固性聚合物组成的组中选出的。
4、依据权利要求3的一种容器，其中，所述的填料是低碳钢。
5、依据权利要求1的一种容器，还包括一个二次空气进气管，它位于反应器进口和出口之间。
6、依据权利要求5的一种容器，其中，二次空气进口位于至少一个室的下游并位于至少一个室的上游。
7、依据权利要求6的一种系统，其中，二次空气进口提供高达约15%的二次空气进口下游处的体积流量。
8、依据权利要求8的一种系统，其中，二次空气进口提供约2至4%的二次空气进口下游端的体积流量。
9、依据权利要求1的一种系统，其中，还包括一位于邻近催化剂收集器的一个出口处的一个氧化催化剂源。
10、依据权利要求9的一种系统，其中，氧化催化剂从下组中选择：该组包括铁、铜和它们的氧化物。
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CA2130811A1 (en) 1993-09-02
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AU3731093A (en) 1993-09-13
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AU664884B2 (en) 1995-12-07
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WO1993016785A1 (en) 1993-09-02
BR9305969A (pt) 1997-10-21

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