CN101454081A - NOx还原催化剂、NOx还原催化剂系统、及NOx还原方法 - Google Patents
NOx还原催化剂、NOx还原催化剂系统、及NOx还原方法 Download PDFInfo
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Abstract
本发明公开一种用于还原处理气体中的NOx的NOx还原催化剂,其特征在于其包含:含有氧化物的催化剂载体、NOx吸收组分和NOx净化组分。
Description
技术领域
本发明涉及将汽车排气和发电厂的烟道气中所含的氮氧化物还原的NOx还原催化剂、NOx还原催化剂系统、及NOx还原方法。
背景技术
汽车排气和发电厂的烟道气含有有害的氮氧化物(NOx)。已经开发出选择性还原这些NOx的催化剂(以下称为SCR催化剂)。例如,公开了使用SCR催化剂将柴油机排气中所含的NOx还原为N2的技术,该SCR催化剂包括用铁和镧进行了离子交换的β型沸石(参见专利文献1)。
专利文献1:特开2005-177570号公报
发明内容
发明所要解决的技术问题
然而,常规的SCR催化剂的NOx还原性能在200℃或更低的低温下会显著下降。因此,存在常规的SCR催化剂不能充分降低低温处理气体如柴油机排气中的NOx的问题。
本发明针对上述问题作出。本发明的一个目的是提供即使在低温下也表现出高的NOx处理性能的NOx还原催化剂、NOx还原催化剂系统、和NOx还原方法。
解决问题的技术方案
(1)根据权利要求1的本发明提供还原处理气体中的NOx的NOx还原催化剂,其包含:含有氧化物的催化剂载体;NOx吸收组分(component);和NOx净化组分。
本发明的NOx还原催化剂在低温范围(例如在200℃或更低的温度下)通过NOx吸收组分吸收NOx。在较高的温度范围(例如在高于200℃的温度下),NOx吸收组分释放所吸收的NOx。释放的NOx通过在高温下活化的NOx净化组分还原。在高温下活化的NOx净化组分不仅还原由NOx吸收组分吸收的NOx,而且还还原新流入的处理气体中的NOx。因此,本发明的NOx还原催化剂可以在从低温到高温的宽温度范围内净化NOx,非常实用。
所述处理气体的实例为:汽车发动机(例如,汽油发动机、柴油发动机等)排放的排气和发电厂的烟道气等。
氧化物的实例为Al2O3、TiO2、ZrO2、沸石等,它们可单独使用、或者两种或更多种组合使用。
NOx吸收组分与具有NOx吸收性能的组分大致相当。NOx吸收组分的实例为碱金属、碱土金属、稀土等,更具体地,为K、Ba、Ce、Nd、Pd、Li等,它们可单独使用、或者两种或更多种组合使用。NOx吸收组分的混合量优选在0.05~2mol/L的范围内。
NOx净化组分与可以由NOx和氨生成氮气和水的组分大致相当。NOx净化组分的实例为V、Fe、Ce、La等,它们可单独使用、或者两种或更多种组合使用。NOx净化组分的混合量优选在0.1~3mol/L的范围内。NOx吸收组分与NOx净化组分的混合量比(重量比)优选在1:0.5~20的范围内,更优选在1:1~15的范围内。在混合了可以既是NOx吸收组分同时也是NOx净化组分的物质(例如Ce)的情形中,假设经离子交换的沸石中的Ce为NOx净化组分,并假设其它的Ce为NOx吸收组分,以计算NOx吸收组分与NOx净化组分的混合量比(重量比)。
本发明的NOx还原催化剂在全部或部分催化剂中可含有混合状态的NOx吸收组分和NOx净化组分。或者,NOx还原催化剂可分别包括其中不均匀地分布有NOx吸收组分的部分和其中不均匀地分布有NOx净化组分的部分。其中不均匀地分布有NOx吸收组分的部分是其中NOx吸收组分的浓度高于其它区域的部分,更优选地是含有基本上全部NOx吸收组分的部分。优选的是,其中不均匀地分布有NOx吸收组分的部分基本上不含NOx净化组分。其中不均匀地分布有NOx净化组分的部分是其中NOx净化组分的浓度高于其它区域的部分,更优选地是含有基本上全部NOx净化组分的部分。优选的是,其中不均匀地分布有NOx净化组分的部分基本上不含NOx吸收组分。
本发明的NOx还原催化剂可含有作为其它组分的贵金属(例如,Pt、Rh、Pd、Ru、Ir、Au、Ag等)。贵金属的混合量优选在0.1~3.0g/L的范围内。混合0.1g/L或更多的贵金属对于净化处理气体中除NOx以外的有害组分(例如,HC和CO)是高效的。混合3.0g/L或更少的贵金属不妨碍NOx吸收组分和NOx净化组分的效果。
贵金属可以与,例如,NOx吸收组分、NOx净化组分、或这两者混合。贵金属可混合到其中基本上既不存在NOx吸收组分也不存在NOx净化组分的部分中。在这种情形中,包含贵金属的部分可位于,例如,处理气体流动方向上、含有NOx吸收组分和NOx净化组分的部分的下游。
(2)根据权利要求2的本发明提供如权利要求1所述的NOx还原催化剂,其具有包括以下层的层状结构:其中不均匀地分布有NOx吸收组分的A层,和其中不均匀地分布有NOx净化组分的B层。
本发明的NOx还原催化剂在低温下通过其中不均匀地分布有NOx吸收组分的A层吸收NOx。该NOx还原催化剂在高温下从A层释放NOx。释放的NOx到达B层并在B层中被还原,所述B层不均匀地分布有NOx净化组分。
对于A层与B层之间的位置关系,其中A层为上层而B层为下层的结构,或者其中A层为下层而B层为上层的结构均是可接受的。更优选的结构具有A层作为下层而B层作为上层。在该情形中,被下面的A层(其中不均匀地分布有NOx吸收组分的层)暂时吸收后释放的NOx必然通过上面的B层(其中不均匀地分布有NOx净化组分的层)而在该B层中净化。因此,NOx净化性能更高。
不均匀地分布有NOx吸收组分的意思是,例如,NOx吸收组分在A层中的浓度高于其在除A层以外的部分中的浓度。优选的是,NOx吸收组分基本上仅存在于A层中并且在A层中基本上不存在NOx净化组分。不均匀地分布有NOx净化组分的意思是,例如,NOx净化组分在B层中的浓度高于其在除B层以外的部分中的浓度。优选的是,NOx净化组分基本上仅存在于B层中并且在B层中基本上不存在NOx吸收组分。
层状结构可为包括A层和B层的两层结构。或者,层状结构可在A层和B层之间、A层和B层之上或之下包括其它层。A层的厚度优选在1~150μm的范围。B层的厚度优选在1~150μm的范围。A层与B层的层厚度之比优选在1:1~10的范围。
(3)根据权利要求3的本发明提供如权利要求1所述的NOx还原催化剂,其具有上游部分和下游部分沿着处理气体的流动方向顺次布置的结构,所述上游部分中不均匀地分布有所述NOx吸收组分,并且所述下游部分中不均匀地分布有所述NOx净化组分。
本发明的NOx还原催化剂在低温下通过其中不均匀地分布有NOx吸收组分的上游部分吸收NOx,并且在高温下从该上游部分释放NOx。该释放的NOx随着处理气体的流动而到达下游部分并在其中被还原,所述下游部分中不均匀地分布有NOx净化组分。即,在本发明的NOx还原催化剂中,被上游部分暂时吸收后释放的NOx可以通过其中不均匀地分布有NOx净化组分的下游部分,因此,NOx净化性能更高。
不均匀地分布有NOx吸收组分的意思是,例如,NOx吸收组分在上游部分中的浓度高于其在除上游部分以外的部分中的浓度。优选的是,NOx吸收组分基本上仅存在于上游部分中并且在上游部分中基本上不存在NOx净化组分。不均匀地分布有NOx净化组分的意思是,例如,NOx净化组分在下游部分中的浓度高于其在除下游部分以外的部分中的浓度。优选的是,NOx净化组分基本上仅存在于下游部分中并且在下游部分中基本上不存在NOx吸收组分。
本发明的NOx还原催化剂可仅包括所述上游部分和所述下游部分。或者,NOx还原催化剂可在上游部分的上游侧上、在上游部分与下游部分之间、或在下游部分的下游侧上包括其它部分。
上游部分与下游部分的长度之比优选在1:0.1~10的范围内。
在本发明的NOx还原催化剂中,例如,如图3所示,下游部分11和上游部分15可为单独的主体,其中下游部分11的催化剂层9和上游部分15的催化剂层13分别形成在单独的基材7的表面上。或者,本发明的NOx还原催化剂将单一基材的表面分隔,并在其上形成上游部分和下游部分。
(4)根据权利要求4的本发明提供如权利要求1至3中任一项所述的NOx还原催化剂,其中在整个NOx还原催化剂中所述NOx吸收组分与所述NOx净化组分的重量比在1:0.1~20的范围内。
在本发明的NOx还原催化剂中,NOx净化组分与NOx吸收组分的重量比为0.1或更大(更优选0.5或更大)。因此,可以抑制NOx的过度吸收。而且,由于NOx净化组分与NOx吸收组分的重量比为20或更小(更优选15或更小),吸收的NOx可以充分净化。
(5)根据权利要求5的本发明提供如权利要求1至4中任一项所述的NOx还原催化剂,其中所述NOx吸收组分选自碱金属、碱土金属和稀土。
由于本发明的NOx还原催化剂的NOx吸收组分选自以上物质,因此NOx净化性能更高。
(6)根据权利要求6的本发明提供如权利要求1至5中任一项所述的NOx还原催化剂,其中所述NOx净化组分为选自V、Fe、Ce和La中的一种或多种。
由于本发明的NOx还原催化剂的NOx净化组分为以上物质中的一种或多种,因此NOx净化性能更高。
(7)根据权利要求7的本发明提供如权利要求1至6中任一项所述的NOx还原催化剂,其中所述氧化物为选自Al2O3、TiO2、ZrO2和沸石中的一种或多种。
由于本发明的NOx还原催化剂的氧化物为以上物质中的一种或多种,因此NOx净化性能更高。
(8)根据权利要求8的本发明提供如权利要求1至7中任一项所述的NOx还原催化剂用于净化汽车排气的用途。
本发明的NOx还原催化剂能净化排气中的NOx。
(9)根据权利要求9的本发明提供NOx还原催化剂系统,其包括:如权利要求1至8中任一项所述的NOx还原催化剂,以及向供应至NOx还原催化剂的所述处理气体添加氨源的氨源添加设备。
本发明的NOx还原催化剂系统可以使用通过氨源添加设备添加的氨源来还原NOx。即,本发明的NOx还原催化剂系统可以在NOx净化组分的存在下通过所谓的SCR方法使NOx和氨相互反应,从而将NOx还原为氮气。
氨源与结果产生氨的物质大致相当。氨源的实例为氨、尿素水溶液、和铵化合物等。
氨源添加设备与可以将氨源添加至处理气体的设备大致相当。在氨源为液体的情形中,氨源添加设备的实例为注射器等。
在NOx净化组分难以引起NOx还原反应的条件下,例如,当处理气体和NOx还原催化剂的温度低(例如200℃或更低)时,氨源添加设备,例如,可以停止氨源的供应或降低其供应量。以这种方式,可以抑制氨源的使用量。而且,可以减少未反应的、残留在处理气体中的氨的量。
(10)根据权利要求10的本发明提供NOx还原催化剂系统,其包括:如权利要求1至8中任一项所述的NOx还原催化剂,以及使供应至NOx还原催化剂的排气达到富态的富态实现设备。
在本发明的NOx还原催化剂系统中,通过富态实现设备将供应至如权利要求1至8中任一项所述的NOx还原催化剂的处理气体控制为富态,从而净化排气中的NOx。
富态实现设备的实例为向处理气体中添加燃料(轻油、汽油等)的设备。在处理气体为内燃机排气的情况下的富态实现设备的其它实例为改变内燃机的运转条件以改变排气组成的设备;以及通过补充喷射、向排气体系中添加HC、富掺料(rich spike)和硫再生而利用处于富态的排气的设备。
所述富态是指与化学计量态相比燃料过量的状态。例如,当处理气体为汽油发动机的排气时,空气-燃料比为14.6或更小;当处理气体为柴油发动机的排气时,空气-燃料比为14.5或更小。
对所述富态持续的时间没有限制。该时间可为约0.1秒的尖峰状(spike-like)时间,或为如数小时的长时间。富态和其它状态的模式可为,例如,如图6和7所示,在某时间在富态与其它状态的区间之间周期性切换,并且可使得各区间中的气体-燃料比恒定。或者,如图8所示,可周期性地逐渐(例如,按照正弦曲线)改变空气-燃料比以产生富态。
(11)根据权利要求11的本发明提供通过如权利要求1至8中任一项所述的NOx还原催化剂来还原处理气体中所含的NOx的NOx还原方法。
本发明的NOx还原方法能在从低温到高温的宽温度范围内净化NOx,实用性高。
附图说明
[图1]是显示NOx还原催化剂5的结构的横截面图。
[图2]是显示NOx还原催化剂5的结构的横截面图。
[图3]是显示NOx还原催化剂5的结构的横截面图。
[图4]是显示实验系统的结构的简图。
[图5]是显示实验系统的结构的简图。
[图6]是显示排气17的组成变化的说明图。
[图7]是显示排气17的组成变化的说明图。
[图8]是显示排气17的组成变化的说明图。
[图9]是显示实验系统的结构的简图。
[图10]是显示实验系统的结构的简图。
符号说明
1、7...陶瓷蜂窝
3...催化剂层
3a...下层部分
3b...上层部分
5...NOx还原催化剂
9...下游催化剂层
11...下游催化剂
13...上游催化剂层
15...上游催化剂
17...排气
19...发动机
21...注射器
23、25...排气分析仪
27...柴油发动机
29...排气管
30...轻油
31...轻油添加设备
33...控制设备
具体实施方式
将基于实施例对本发明进行说明。
实施例1
将下列组分混合,搅拌1小时,之后,使用球磨机湿式粉碎1小时。
沸石β(二氧化硅/氧化铝比为35),Tosoh Corporation制造:100重量份
硝酸铁:25重量份
γ氧化铝:20重量份
乙酸钡:25重量份
离子交换水:200重量份
之后,进一步加入10重量份(换算为Al2O3)作为粘合剂的氧化铝溶胶(AS200,Nissan Chemical Industries,Ltd.制造)以制备浆料。
将上述浆料涂布于NGK Insulators,Ltd.制造的陶瓷蜂窝1(密度为300个孔/平方英寸,壁厚为8密耳,尺寸为Φ190.5×L76mm,容积为2.2L)。将多余的浆料吹掉后,将陶瓷蜂窝1在200℃下干燥1小时,并在500℃下煅烧1小时,从而制造如图1所示的具有催化剂层3的NOx还原催化剂5。催化剂层3中Fe和Ba各自的量为0.15mol/L和0.1mol/L。
表1显示了实施例1、和后述实施例2至10以及比较例1至5中制造的NOx还原催化剂的催化剂层的组成。
[表1]
※实施例7、9和10中Pt、Rh和Pd的量的单位为g/L。
实施例2
以与实施例1中相同的方式制造NOx还原催化剂5,不同之处在于:用相同量的Tosoh Corporation制造的ZSM5(二氧化硅/氧化铝比为30)代替沸石β使用。
实施例3
以与实施例1中相同的方式制造NOx还原催化剂5,不同之处在于:用含有氧化钒的草酸水溶液代替硝酸铁使用。钒氧化物的草酸水溶液的量为催化剂层3中含有0.2mol/L钒的量。
实施例4
以与实施例1中相同的方式制造NOx还原催化剂5,不同之处在于:用硝酸铈代替硝酸铁使用。硝酸铈的量为催化剂层3中含有0.2mol/L铈的量。
实施例5
以与实施例1中相同的方式制造NOx还原催化剂5,不同之处在于:用硝酸镧代替硝酸铁使用。硝酸镧的量为催化剂层3中含有0.2mol/L镧的量。
实施例6
以与实施例1中相同的方式制造NOx还原催化剂5,不同之处在于:用乙酸钾代替乙酸钡使用。乙酸钾的量为催化剂层3中含有0.1mol/L钾的量。
实施例7
以与实施例1中相同的方式制造NOx还原催化剂5,不同之处在于:用乙酸钾、乙酸锂、硝酸铈和硝酸钯代替乙酸钡使用。硝酸铈的量为催化剂层3中含有0.2mol/L铈的量,且硝酸钯的量为催化剂层3中含有1g/L钯的量。乙酸钾和乙酸锂各自的量为催化剂层3中含有0.1mol/L钾和0.1mol/L锂的量。
实施例8
以与实施例1中相同的方式制造NOx还原催化剂,不同之处在于:用硝酸钕代替乙酸钡使用。乙酸钕的量为催化剂层3中含有0.1mol/L钕的量。
实施例9
将下列组分混合,搅拌1小时,之后,使用球磨机湿式粉碎1小时。
沸石β(二氧化硅/氧化铝比为35),Tosoh Corporation制造:100重量份
硝酸铁:25重量份
离子交换水:250重量份
之后,进一步加入5重量份(换算为Al2O3)作为粘合剂的氧化铝溶胶(AS200,Nissan Chemical Industries,Ltd.制造)以制备浆料A。
而且,将下列组分混合,搅拌1小时,之后,使用球磨机湿式粉碎1小时。
γ氧化铝:20重量份
乙酸钡:25重量份
离子交换水:50重量份
之后,进一步加入3重量份(换算为Al2O3)作为粘合剂的氧化铝溶胶(AS200,Nissan Chemical Industries,Ltd.制造)以制备浆料B。
首先将浆料B涂布于与实施例1中同样的陶瓷蜂窝1上。之后,将陶瓷蜂窝1在250℃下干燥1小时,浸渍在二硝基二氨基铂水溶液和氯化铑水溶液中以吸收Pt和Rh,并在350℃下干燥,以形成如图2所示的下层部分3a。Pt和Rh的担载量分别为2g/L和0.5g/L。随后,涂布浆料A以形成上层部分3b。将陶瓷蜂窝1在500℃下煅烧1小时,从而制造具有两层结构的NOx还原催化剂5,其中催化剂层3由下层部分3a和上层部分3b构成。
在催化剂层3中,仅上层部分3a含有Fe,且仅下层部分3b含有Ba。整个催化剂层3中Fe和Ba的量分别为0.15mol/L和0.1mol/L。
实施例10
准备两个基材,即NGK Insulators,Ltd.制造的陶瓷蜂窝7(密度为300个孔/平方英寸,壁厚为8密耳,尺寸为Φ190.5×L38mm,容积为1.1L),它们分别具有实施例1中所使用的陶瓷蜂窝1一半的催化剂长度和容积。
将浆料A涂布于一个陶瓷蜂窝7上。将陶瓷蜂窝7干燥并煅烧,从而制造如图3所示的具有下游催化剂层9的下游催化剂11。干燥和煅烧的条件与实施例1中的相同。下游催化剂层9中Fe的量为0.15mol/L。
而且,将浆料B涂布于另一个陶瓷蜂窝7上。贵金属以与实施例9中相同的方式担载。干燥并煅烧该陶瓷蜂窝7,从而制造如图3所示的具有上游催化剂层13的上游催化剂15。干燥和煅烧的条件与实施例1中的相同。上游催化剂层13中Ba的量为0.1mol/L。Pt和Rh的担载量分别为2g/L和0.5g/L。
相对于排气(处理气体)的流动,将上游催化剂15和下游催化剂11顺次布置使得上游催化剂15位于上游侧而下游催化剂11位于下游侧,从而形成由这两种催化剂构成的NOx还原催化剂5。
(比较例1)
如下制造用作固定式脱硝催化剂的V2O5/TiO2-WO3催化剂。
将下列组分混合、搅拌并使用球磨机粉碎1小时以制备浆料。
含有5wt%氧化钨的氧化钛(比表面积82m2/g):100重量份
Ishihara Sangyo Kaisha Ltd.制造的氧化钛溶胶:20重量份(换算为TiO2)
离子交换水:100重量份
施用上述浆料涂布与实施例1中同样的陶瓷蜂窝以形成催化剂层,并进一步将其以与实施例1中相同的方式干燥和煅烧。催化剂层的涂布量为120g。
随后,将上述催化剂层浸渍到含有V的水溶液中,该水溶液通过将V2O5溶解到80℃的草酸水溶液中而制备。在从含有V的水溶液中取出后,吹掉多余的水滴。之后,将催化剂层在100℃下干燥并在500℃下煅烧1小时从而在催化剂层的表面上形成氧化钒。催化剂层上V的担载量为0.2mol/L。
(比较例2)
将下列组分混合以制备浆料。
用Fe进行了离子交换的沸石β:100重量份
氧化铝溶胶:10重量份(换算为氧化铝)
离子交换水:50重量份
施用上述浆料涂布与实施例1中同样的陶瓷蜂窝,将其干燥并煅烧以制造催化剂。
(比较例3)
以与实施例1中相同的方式制造催化剂,不同之处在于:未将γ氧化铝和乙酸钡混入浆料。
(比较例4)
以与实施例1中相同的方式制造催化剂,不同之处在于:未将硝酸铁混入浆料。
(比较例5)
以与实施例9中相同的方式制造催化剂,不同之处在于:未涂布浆料B。即,在比较例5中,将浆料A直接涂布于陶瓷蜂窝上以形成催化剂层,将其干燥并煅烧从而制造仅具有由浆料A制备的催化剂层的催化剂。
实施例11
a)催化剂的耐久性
使用电炉,在含有10体积%水蒸气的气氛中对实施例1至10中制造的NOx还原催化剂5和比较例1至5中制造的催化剂进行800℃、10小时的水热耐久性试验。
b)实验系统的制作
在上述a)的耐久性试验后,制造如图4所示的实验系统,其包括:催化剂5(实施例1至10中制造的NOx还原催化剂5或比较例1至5中制造的催化剂);具有涡轮中间冷却器(turbointercooler)的6.6L排量发动机19,其将排气17供应至催化剂5;注射器21(氨源添加设备),其将30%尿素水溶液18喷雾至催化剂5上游的排气17中;排气分析仪23,其测量催化剂5上游的排气17中的NOx浓度;以及排气分析仪25,其测量催化剂5下游的排气17中的NOx浓度。两个排气分析仪23和25均为Horiba,Ltd.制造的MEXA7000。
c)NOx净化性能的评价
在上述b)的实验系统中,运转发动机9,并且将排气17供应至催化剂5。当排气17的温度为200℃或更高时,将30%尿素水溶液18通过注射器21喷雾至排气17中。主要设定条件如下。
发动机9的燃料:具有10ppm或更少的S(硫)的市售轻油
发动机9的转速:1600rpm,恒定
催化剂5的排气处理量:30,000/小时
30%尿素水溶液的添加量:与换算为氨的排气17中的NOx量等摩尔的量(当排气17的温度为200℃或更低时,不进行添加。)
通过改变发动机9的负荷调节排气17的温度,并且先将该温度设为150℃恒定。当排气17的温度达到150℃时,等待3分钟直至排气17的状态稳定。然后,通过排气分析仪23测量在进入催化剂5之前排气17中的NOx浓度C1(ppm)。还通过排气分析仪25测量由催化剂5放出的排气17中的NOx浓度C2(ppm)。
随后,将排气17的温度设为250℃恒定。以与上述相同的方式,在排气17的温度达到250℃之后,等待3分钟,并且测量在进入催化剂5之前排气17中的NOx浓度C1(ppm)以及由催化剂5放出的排气17中的NOx浓度C2(ppm)。
而且,将排气17的温度设为350℃恒定。以与上述相同的方式,在排气17的温度达到350℃之后,等待3分钟,并且测量进入催化剂5之前排气17中的NOx浓度C1(ppm)以及由催化剂5放出的排气17中的NOx浓度C2(ppm)。然后,根据下式(1)计算排气温度17为150℃、250℃、和350℃的各情形中的NOx净化率(%)。
式(1):NOx净化率(%)=((C1-C2)/C1)×100
[表2]
如以上表2所示,实施例1至10中制造的NOx还原催化剂5在任何温度的排气17下均表现出非常高的NOx净化率。相反,比较例1至5的催化剂在排气17的温度为150℃和250℃时表现出非常低的NOx净化率。
实施例12
a)以与实施例11的a)中相同的方式,在含有10体积%水蒸气的气氛中对实施例1至10中制造的NOx还原催化剂5和比较例1至5中制造的催化剂进行800℃、10小时的水热耐久性试验。
b)实验系统(催化剂系统)的结构
如图5所示,制造实验系统35,其包括:催化剂5(实施例1至10中制造的NOx还原催化剂5或比较例1至5中制造的催化剂);2L排量的柴油发动机27,其将排气17供应至催化剂5;从柴油发动机27延伸至催化剂5的排气管29;轻油添加设备31,其将轻油30添加至排气管29;排气分析仪23,其测量催化剂5上游的排气17中的NOx浓度;以及排气分析仪25,其测量催化剂5下游的排气17中的NOx浓度。轻油添加设备31包括储存轻油的轻油罐37;注射器39,其将轻油注入排气管29中;轻油供给管41,其将从轻油罐取出的轻油供给至注射器39;以及控制器43,其控制注射器39中轻油的注射量。
c)NOx净化性能的评价
在上述b)的实验系统中,运转柴油发动机27,并且将排气17供应至催化剂5。将柴油发动机27的转速设为2100rpm。催化剂5入口处的温度控制为250℃。
对于排气17的组成,将A/F比基本设为30,如图6所示。然而,通过轻油添加设备31向排气17间歇添加轻油使得其中A/F比为14.2的状态可在30秒的时间间隔内出现1秒。
当排气17的温度达到250℃时,等待3分钟直至排气17的状态稳定。然后,通过排气分析仪23测量在进入催化剂5之前排气17中的NOx浓度C1(ppm)。还通过排气分析仪25测量通过催化剂5的排气17中的NOx浓度C2(ppm)。
NOx净化率(%)根据上式(1)计算。结果如表3所示
[表3]
如以上表3所示,实施例1至10中制造的NOx还原催化剂5表现出非常高的NOx净化率。相反,比较例1至5的催化剂表现出非常低的NOx净化率。
实施例13
将通过图9对催化剂系统46的结构进行说明。在催化剂系统46中,将实施例10中所述的NOx还原催化剂5装入排气管45的内部。将上游催化剂15装入排气管45的上游侧,并将下游催化剂11装入排气管45的下游侧。排气管45在装入了上游催化剂15的部分与装入了下游催化剂11的部分之间具有窄部分47,该窄部分47具有小的横截面。而且,排气管45的上游催化剂15的上游侧和下游催化剂11的下游侧具有比装入了上游催化剂15和下游催化剂11的部分更小的横截面。
在催化剂系统46中,将注射尿素水溶液的注射器49安装在上述窄部分47上。通过注射器49,可以将尿素水溶液添加到供应至下游催化剂11的排气中。使用泵53将储存在尿素水溶液罐51中的尿素水溶液通过导管55供应至注射器49。从注射器49注射的尿素水溶液的量通过控制器57控制。
如果装入排气管45的NOx还原催化剂,如实施例1至9的NOx还原催化剂一样,是一体型的而未分离成上游催化剂和下游催化剂,则供应尿素水溶液的注射器49可设置在NOx还原催化剂的上游侧(例如,图9中的位置A)。
实施例14
将通过图10对催化剂系统46的结构进行说明。在催化剂系统48中,将实施例10中所述的NOx还原催化剂5装入排气管45的内部。将上游催化剂15装入排气管45的上游侧,并将下游催化剂11装入排气管45的下游侧。排气管45在装入了上游催化剂15的部分与装入了下游催化剂11的部分之间具有窄部分47,该窄部分47具有小的横截面。而且,排气管45的上游催化剂15的上游侧和下游催化剂11的下游侧具有比装入了上游催化剂15和下游催化剂11的部分更小的横截面。
在催化剂系统48中,将注射轻油的注射器59安装在排气管45的上游催化剂15的上游位置。通过注射器59,可以将轻油添加到供应至上游催化剂15的排气中,从而使排气达到富态。
应当理解,本发明不应限于上述实施例,而是可在不背离本发明的范围内以各种形式实施。
例如,NOx吸收组分与NOx净化组分在整个NOx还原催化剂5中的重量比不限于实施例中的值。该重量比可在1:0.1~20的范围内。在该情形中也可以获得相同的效果。
各实施例的NOx还原催化剂5中的氧化物可为TiO2或ZrO2。在该情形中也可以获得相同的效果。
在实施例10中,可将单个陶瓷蜂窝1分隔成上游部分和下游部分。浆料B可施用至上游部分且浆料A可施用至下游部分。以这种方式,上游催化剂层13和下游催化剂层9可以形成在单个陶瓷蜂窝1的表面上。
Claims (11)
1.一种还原处理气体中的NOx的NOx还原催化剂,其包含:
含有氧化物的催化剂载体;
NOx吸收组分;和
NOx净化组分。
2.根据权利要求1的NOx还原催化剂,其具有包括以下层的层状结构:
其中不均匀地分布有所述NOx吸收组分的A层,和
其中不均匀地分布有所述NOx净化组分的B层。
3.根据权利要求1的NOx还原催化剂,其具有其中上游部分和下游部分沿着所述处理气体的流动方向顺次布置的结构,所述上游部分中不均匀地分布有所述NOx吸收组分,所述下游部分中不均匀地分布有所述NOx净化组分。
4.根据权利要求1至3中任一项的NOx还原催化剂,其中在整个NOx还原催化剂中所述NOx吸收组分与所述NOx净化组分的重量比在1:0.1~20的范围内。
5.根据权利要求1至4中任一项的NOx还原催化剂,其中所述NOx吸收组分选自碱金属、碱土金属和稀土。
6.根据权利要求1至5中任一项的NOx还原催化剂,其中所述NOx净化组分为选自V、Fe、Ce和La中的一种或多种。
7.根据权利要求1至6中任一项的NOx还原催化剂,其中所述氧化物为选自Al2O3、TiO2、ZrO2和沸石中的一种或多种。
8.根据权利要求1至7中任一项的NOx还原催化剂,其用于净化汽车排气的用途。
9.一种NOx还原催化剂系统,包含:
根据权利要求1至8中任一项的NOx还原催化剂;以及
向供应至所述NOx还原催化剂的处理气体添加氨源的氨源添加设备。
10.一种NOx还原催化剂系统,包含:
根据权利要求1至8中任一项的NOx还原催化剂;以及
使供应至所述NOx还原催化剂的处理气体达到富态的富态实现设备。
11.一种NOx还原催化剂方法,其使用权利要求1至8中任一项的NOx还原催化剂还原所述处理气体中所含的NOx。
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2007
- 2007-05-17 KR KR1020087029240A patent/KR101052655B1/ko not_active IP Right Cessation
- 2007-05-17 US US12/302,301 patent/US20090196811A1/en not_active Abandoned
- 2007-05-17 CN CN201510217075.XA patent/CN104959035A/zh active Pending
- 2007-05-17 EP EP07743570.9A patent/EP2025401B1/en active Active
- 2007-05-17 CN CNA2007800198858A patent/CN101454081A/zh active Pending
- 2007-05-17 WO PCT/JP2007/060135 patent/WO2007138874A1/ja active Application Filing
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Also Published As
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KR101052655B1 (ko) | 2011-07-29 |
CN104959035A (zh) | 2015-10-07 |
EP2025401A1 (en) | 2009-02-18 |
KR20090017554A (ko) | 2009-02-18 |
JP5373255B2 (ja) | 2013-12-18 |
EP2025401B1 (en) | 2018-10-31 |
JP2007313486A (ja) | 2007-12-06 |
WO2007138874A1 (ja) | 2007-12-06 |
EP2025401A4 (en) | 2014-04-30 |
US20130058841A1 (en) | 2013-03-07 |
US20090196811A1 (en) | 2009-08-06 |
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