CN1353006A - 选择性催化还原氮氧化物的废气处理装置及其废气处理方法 - Google Patents
选择性催化还原氮氧化物的废气处理装置及其废气处理方法 Download PDFInfo
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Abstract
本发明提供了一种在贫油燃烧产生的废气条件下选择性催化还原氮氧化物的废气处理装置,其含有至少一种带有催化活性组分的用于选择性催化还原的催化剂(SCR组分)。废气处理装置的特征在于催化剂除了SCR组分之外,还含有至少一种氮氧化物的储存组分(NOx组分)。
Description
本发明提供了一种在贫油燃烧产生的废气(lean exhaust gas)条件下选择性催化还原氮氧化物的废气处理装置,其含有至少一种带有催化活性组分的用于选择性催化还原的催化剂(SCR组分)。
发电站的固定燃烧装置和柴油发动机以及贫油运行(leanoperated)的汽油发动机内排放出富含氧气的废气,该废气含有作为有害物质的未燃烧的碳氢化合物(HC)、一氧化碳(CO)和氮氧化物(NOX)。为了从贫油燃烧产生的废气中除去氮氧化物,所谓的选择性催化还原(SCR)方法的利用在发电站业界已经进行了很长时间。在此,将氨(NH3)引入到废气中,借助适当的催化剂氨与氮氧化物选择性反应生成氮气和水。在固定操作条件下,利用该方法氮氧化物可以得到大于80%的转化率。
由于立法要求降低汽车中氮氧化物排放(在欧洲到2005和2008分别是EURO IV和EURO V,在美国到2007分别是LEV II),特别是在载重汽车的情况下,SCR技术的应用变得越来越迫切。由于氨的高毒性和挥发性,所以在汽车的移动式应用中使用经适当处理能释放出氨的无毒前体化合物。优选使用水溶液形式的脲。为了水解脲,在两步反应中使用将脲溶液水解成氨和二氧化碳的所谓水解催化剂。在废气处理装置内水解催化剂位于SCR催化剂的上游。借助于特殊的计量系统在水解催化剂的上游将脲溶液注入到废气流中。
该类废气处理的缺点在于脲的水解和利用现代SCR催化剂的选择性催化还原都在高于160-200℃的条件下开始。因此,在废气温度低于该温度范围的内燃机运行条件下,发动机产生的氮氧化物以未改变的形式通过废气处理装置,并释放到环境中。现代的脲计量系统考虑了该事实并只有当废气温度高于170℃时才将脲溶液注入到废气流中。
本发明的目的是提供一种废气处理装置,该装置能够减少来自贫油运行内燃机甚至是废气温度低于用于脲水解和选择性催化还原的点火温度的操作条件下氮氧化物的排放。本发明的另一个目的是提供一种通过使用氨的选择性催化还原来除去内燃机贫油燃烧产生的废气中氮氧化物的方法。
通过在贫油燃烧产生的废气条件下用于选择性催化还原的氮氧化物的废气处理装置来实现该目的,其含有至少一种具有催化活性组分的用于选择性催化还原(SCR组分)的催化剂。废气处理装置的特征在于除了SCR组分之外,催化剂还含有至少一种用于储存氮氧化物的组分(NOX储存组分)。
在下面,催化剂的点火温度可以理解成在催化剂上催化反应进行至50%的转化率时的温度。这样,水解催化剂具有脲水解的点火温度,SCR催化剂具有氮氧化物转化的点火温度。
根据本发明,目的是将废气中存在的氮氧化物在低废气温度时借助于NOX储存组分暂时储存在SCR催化剂上,然后在高温下又释放出来。废气中局部过量的氨便利于氮氧化物的释放,在SCR反应中储存的氮氧化物直接与氨反应。这还意味着如果存在稍微过量的氨或脲溶液,作为氨的下降它们就不会离开SCR体系以及废气装置,但是其与吸附的氮氧化物反应并被氧化成氮气。相应地,在SCR催化剂中NOX储存组分的作用可以比作为三元净化器催化剂中氧气储存材料。
催化剂中的SCR组分可以含有二氧化钛和钒的固体酸体系。此外,固体酸体系可能含有至少一种选自氧化钨(WO3)、氧化钼(MoO3)、二氧化硅、硫酸盐和沸石的组分,其中沸石以酸性H的形式存在或者可以与金属离子进行交换。另外,SCR组分含有至少一种沸石,其中沸石是酸性H的形式或者可以与金属离子进行交换。这些材料因其酸性而能够储存氨。在强烈变化的发动机负荷下这是有利的。
NOX储存组分优选含有至少一种选自碱金属、碱土金属和铈元素的化合物。这些组分能够通过生成硝酸盐来储存二氧化氮。由于内燃机废气的60-95vol.%由一氧化氮组成(依赖于特定的运行状态),为了提高储存过程的效率,因此建议通过与氧化催化剂接触而将一氧化氮转化成二氧化氮。例如,当NOX储存组分自身被铂族金属铂、钯、铑、铱的至少一种所催化时,这种需要可以得到满足。另外,催化剂可以含有基于载体氧化物的催化活性组分,该载体氧化物选自氧化铝、二氧化硅、氧化铈、氧化锆、氧化钛或其混合氧化物,并被至少一种铂族金属铂、钯、铑、铱所催化。
催化剂可以以设定为整体挤出物的蜂窝结构的形式存在,也就是说,加工催化剂的组分以得到可挤出的组合物,然后挤出生成蜂窝结构。该催化剂完全由催化剂组合物构成,因此也被称作整体催化剂。通常地,蜂窝结构具有两个端面和一个侧面所限定的一般圆柱形的形状。废气的流动通道紧密排列在一起穿过蜂窝结构的横截面,从一个端面通向另一个端面。蜂窝密度定义为每横截面上通道的数目。根据特定的应用,蜂窝密度可以是5-300cm-2。
对于特定的应用,挤出仅有的SCR组分来形成蜂窝结构以及将NOX储存组分以涂层的形式涂覆到流动通道的壁上是有利的。用于此的技术对于本领域的技术人员是公知的。
由于整体催化剂一般只有较低的强度,催化剂,也就是SCR组分和NOX储存组分,优选以涂层的形式涂覆到蜂窝形式的催化惰性载体结构的流动通道的壁上。惰性载体结构优选由堇青石组成。在催化剂的另一个实施方案中,SCR组分和氮氧化物的NOX储存组分以两个独立层的形式涂覆到惰性载体结构上,其中NOX储存组分优选位于直接与惰性载体结构接触的底层,SCR组分位于与废气直接接触的上层。
另外,或者除了具有将一氧化氮氧化成二氧化氮的催化活性组分的催化剂外,氧化催化剂也可以位于废气处理装置内用于选择性催化还原催化剂的上游,其也能将一氧化氮氧化成二氧化氮。根据本发明的NOX储存组分含有非催化的活性铂族金属,在该类废气处理装置的特殊实施方案中优选使用含有氧化催化剂与催化剂上游的结合。在该实施方案中,一氧化氮氧化成氮氧化物仅仅发生在氧化催化剂的上游,该氧化催化剂可以是在氧化铝上含有铂。根据本发明在氧化催化剂上形成的二氧化氮将由催化剂的NOX储存组分所吸附。
如果用于选择性催化还原所需的氨打算由脲水解得到,那么水解催化剂位于废气处理装置内的氧化催化剂和选择性催化还原催化剂之间。使用适当的计量系统将要水解的脲溶液注入到废气流中,计量系统位于氧化催化剂的下游和水解催化剂的上游。在氨大大过量的情况下,不需要的氨可能排放到环境中。为了避免这些排放,可以将所谓的能将氨氧化生成氮气和水的氨阻隔催化剂引入到废气处理装置的SCR催化剂的下游。
利用所述的废气处理装置,下面描述通过使用氨进行选择性催化还原、除去内燃机贫油燃烧产生的废气中氮氧化物的方法。废气通过含有用于进行选择性催化还原的催化活性组分(SCR组分)和氮氧化物的储存组分(NOX储存组分)的催化剂,并至少有偶尔的氨供应。在废气温度低于用于选择性催化还原的组分的点火温度的发动机的运行阶段,存在于废气中的氮氧化物由NOX储存组分所吸附。为了避免将氨排放到环境中,在这些运行阶段将停止氨的引入(要么直接地要么以前体化合物的形式)。在另一方面,在废气的温度高于选择性催化还原的点火温度的情况下,将重新开始氨的供应。作为提高的废气温度和废气中存在的氨的结果,NOX储存组分储存的氮氧化物将进行解吸,并与废气中存在的氮氧化物一起在SCR组分上与催化剂中的氨反应生成氮气和水。
这种功能不同于传统的NOX储存催化剂,其中释放出的氮氧化物在储存组分自身上还原成氮气。根据本发明,释放出的氮氧化物在催化剂的SCR组分上转化成氮气。
在此可以实施的废气处理装置和方法特别适合于柴油发动机的使用。但是,废气处理装置和方法也可用于贫油运行的汽油发动机的贫油燃烧产生的废气处理。这种类型的发动机也包括直接注入式汽油发动机,所谓的GDI发动机。在加速阶段,为了能够提供加速所需的动力,这样的发动机也在富空气/燃油混合物的条件下操作。根据DE 19820 828 A1,这样的阶段适于在适当的催化剂上从废气组分中形成氨。
DE 198 20 828 A1描述了一种用于GDI发动机的废气净化系统。该废气净化系统包括从富油燃烧产生的废气组合物中的各个废气组分产生氨的第一催化剂。用于该反应的适当催化剂是传统的三元催化剂。但是在富油燃烧产生的废气(rich exhaust gas)条件下任何其它的优化用于形成氨的催化剂都可以使用。第一催化剂下游的第二催化剂储存了生成的氨,借助于储存的氨在贫油燃烧产生的废气条件下选择性地还原氮氧化物。对于这样的废气净化系统来说,持续提供足够量的氨来完全还原氮氧化物是很重要的。为了确保上述目的,使用的SCR催化剂具有较高的氨储存能力。
同样地,根据本发明的废气处理装置也可以装备在带有富油燃烧产生的废气的发动机的操作点的条件下能从废气组分中产生氨的催化剂。这种情况下的优点在于催化剂除了具有氨的储存能力,其还具有氮氧化物的储存能力。这提高了发动机的所有操作点平均的氮氧化物的转化。另外,可以减少计量进入废气中的脲溶液的量,甚至是一起省略。
图1-3表示本发明废气处理装置最优选的实施方案。参考数字(1)表示包括废气管(2)和净化室(3)的废气处理装置。在净化室的内部是含有SCR组分和至少一种氮氧化物的储存组分的催化剂(4)。两个实心箭头表示废气进入和离开处理装置。脲作为氨的前体化合物在净化室(3)的前面注入,在催化剂(4)上脲水解产生氨。
图2表示本发明一种更加优选的实施方案。废气处理装置增加了位于第一净化室(3)上游以及脲进入废气流的注入点的上游的第二净化室(5)。该实施方案通过使用在活性氧化铝上含有铂的高活性氧化催化剂而提高了一氧化碳氧化成二氧化氮。由于这样高活性的氧化催化剂也氧化氨,所以其不能与催化剂(4)结合。根据本发明,当带有催化剂的净化室(3)位于低层位置时,该氧化催化剂靠近发动机的出口就会中毒。
在图3的实施方案中净化室(3)还包括催化剂(4)前面的水解催化剂(7)和催化剂(4)下游的氨阻隔催化剂(8)。专用水解催化剂(7)提高了脲的水解生成氨,这样就提高了废气处理装置的总的废气净化效率。这样的水解催化剂在本领域是众所周知的。其可以包括二氧化钛、氧化铝、二氧化硅、氧化锆或其混合氧化物。通过掺合SO3、WO3、Nb2O5和MoO3来稳定和提高该组合物的活性。例如适当的组合物描述在DE 4203807A1中。氨阻隔催化剂(8)通过氧化成氮气和水来阻止氨偶尔进入大气。为了此目的可以使用在活性氧化铝上含有铂的氧化催化剂。
Claims (24)
1.一种用于在贫油燃烧产生的废气条件下选择性催化还原氮氧化物的废气处理装置,其含有至少一种带有催化活性组分的、用于选择性催化还原(SCR组分)的催化剂,其特征在于除了SCR组分催化剂之外,还含有至少一种氮氧化物的存储组分(NOX组分)。
2.根据权利要求1的废气处理装置,其特征在于SCR组分含有二氧化钛和钒的固体酸体系。
3.根据权利要求2的废气处理装置,其特征在于固体酸体系也含有至少一种选自氧化钨、氧化钼、二氧化硅、硫酸盐和沸石的组分,其中沸石以酸性H的形式存在或者可以与金属离子进行交换。
4.根据权利要求1的废气处理装置,其特征在于SCR组分含有至少一种沸石,其中沸石以酸性H的形式存在或者可以与金属离子进行交换。
5.根据权利要求1-4其中之一的废气处理装置,其特征在于NOX储存组分含有至少一种选自碱金属、碱土金属和铈元素的化合物。
6.根据权利要求5的废气处理装置,其特征在于NOX储存组分由至少一种铂族金属铂、钯、铑、和铱所催化。
7.根据权利要求5的废气处理装置,其特征在于催化剂还含有基于载体氧化物的催化活性组分,该载体氧化物选自氧化铝、二氧化硅、氧化铈、氧化锆、氧化钛、或其混合氧化物,并由至少一种铂族金属铂、钯、铑、铱所催化。
8.根据权利要求1的废气处理装置,其特征在于催化剂以设定为整体挤出物的蜂窝结构的形式存在。
9.根据权利要求1的废气处理装置,其特征在于SCR组分以设定为整体挤出物的蜂窝结构的形式存在,在其上以涂层的形式涂覆NOX储存组分。
10.根据权利要求1的废气处理装置,其特征在于氮氧化物的SCR组分和NOX储存组分在蜂窝整体形式的惰性载体结构上以涂层的形式存在。
11.根据权利要求10的废气处理装置,其特征在于氮氧化物的SCR组分和NOX储存组分以两个独立层的形式存在于惰性载体结构上。
12.根据权利要求11的废气处理装置,其特征在于具有NOX储存组分的层直接涂覆到载体结构上,带有SCR组分的层在具有NOX储存组分的层的上面,并直接与废气接触。
13.根据权利要求1的废气处理装置,其特征在于氧化催化剂位于废气处理装置内的选择性催化还原催化剂的上游。
14.根据权利要求13的废气处理装置,其特征在于水解催化剂位于废气处理装置内氧化催化剂和选择性催化还原催化剂之间。
15.根据权利要求14的废气处理装置,其特征在于氨阻隔催化剂位于废气处理装置内选择性催化还原催化剂的下游。
16.一种利用氨的选择性催化还原除去内燃机贫油燃烧产生的废气中氮氧化物的方法,其特征在于废气经过含有用于选择性催化还原的催化活性组分(SCR组分)和氮氧化物的储存组分(NOX组分)的催化剂,同时至少具有偶尔的氨供应,其中当发动机的废气温度低于用于选择性催化还原的组分的点火温度时,NOX储存组分吸附发动机运行阶段废气中的氮氧化物,并且当废气温度高于选择性催化还原的点火温度通过引入氨来解析氮氧化物,在SCR组分上与氨以及氮氧化物进行反应来产生氮气和水。
17.根据权利要求16的方法,其特征在于NOX储存组分被铂族金属铂、钯、铑、铱的至少之一所催化。
18.根据权利要求16或17的方法,其特征在于氧化催化剂位于选择性催化还原催化剂的上游,在氧化催化剂和选择性催化还原催化剂之间向废气中引入氨。
19.根据权利要求18的方法,其特征在于氨阻隔催化剂位于废气处理装置内选择性催化还原催化剂的下游。
20.根据权利要求18的方法,其特征在于水解催化剂位于废气处理装置内的氧化催化剂和选择性催化还原催化剂之间,将通过水解转化成氨的前体化合物供应到水解催化剂以便生成氨。
21.根据权利要求19的方法,其特征在于氨阻隔催化剂位于废气处理装置内的选择性催化还原催化剂的下游。
22.根据权利要求16的方法,其特征在于内燃机是柴油发动机。
23.根据权利要求16的方法,其特征在于内燃机是贫油运行的汽油发动机,其在加速阶段的过程中是在富空气/燃油混合物的条件下工作。
24.根据权利要求23的方法,其特征在于在适当催化剂上把在发动机加速阶段所产生的富油燃烧产生的废气中相应的组分转化成选择性催化还原所需的氨。
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- 2001-11-06 BR BR0105070-2A patent/BR0105070A/pt not_active Application Discontinuation
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KR20020035445A (ko) | 2002-05-11 |
JP2002200413A (ja) | 2002-07-16 |
ZA200109121B (en) | 2002-05-06 |
CA2361029A1 (en) | 2002-05-06 |
US7431895B2 (en) | 2008-10-07 |
AR031734A1 (es) | 2003-10-01 |
DE60144084D1 (de) | 2011-04-07 |
MXPA01011203A (es) | 2004-07-27 |
CN1204960C (zh) | 2005-06-08 |
PL350511A1 (en) | 2002-05-20 |
EP1203611B2 (en) | 2018-10-03 |
BR0105070A (pt) | 2002-06-25 |
EP1203611B1 (en) | 2011-02-23 |
CZ20013917A3 (cs) | 2002-09-11 |
AU8921801A (en) | 2002-05-09 |
ATE499151T1 (de) | 2011-03-15 |
JP4960559B2 (ja) | 2012-06-27 |
RU2278281C2 (ru) | 2006-06-20 |
US20020054844A1 (en) | 2002-05-09 |
EP1203611A1 (en) | 2002-05-08 |
DE10054877A1 (de) | 2002-05-29 |
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