CN102665910B - 蜂窝结构体以及尾气净化装置 - Google Patents

蜂窝结构体以及尾气净化装置 Download PDF

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CN102665910B
CN102665910B CN200980162508.9A CN200980162508A CN102665910B CN 102665910 B CN102665910 B CN 102665910B CN 200980162508 A CN200980162508 A CN 200980162508A CN 102665910 B CN102665910 B CN 102665910B
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exhaust gas
zeolite
cellular unit
gas cleaner
structured body
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CN102665910A (zh
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国枝雅文
吉村健
宫下敏行
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Ibiden Co Ltd
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Ibiden Co Ltd
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Abstract

本发明的蜂窝结构体，具有蜂窝单元，在该蜂窝单元中，包含沸石以及无机粘结剂，并且多个贯穿孔隔着间壁沿长度方向并排设置；在所述蜂窝单元中，仅在从所述长度方向的一方的端部起算长度为全长的1.5％以上20％以下的区域内担载贵金属触媒。

Description

蜂窝结构体以及尾气净化装置
技术领域
本发明涉及一种蜂窝结构体以及具有蜂窝结构体的尾气净化装置。
背景技术
在现有技术中，作为净化汽车尾气的系统之一，熟知的有一种使用氨将NOx还原为氮和水的SCR(Selective Catalytic Reduction)系统。
另外，在SCR系统中，作为吸附氨的材料，熟知的有沸石。
在专利文献1中，作为处理由具备SCR系统的固定燃烧源所产生的尾气的方法，公开了一种方法，即：在SCR系统的下游侧，通过将氨的排出物置于贵金属触媒(催化剂)，在贵金属触媒中使未反应气体氨与氧气进行反应，以生成氮的氧化态更高的反应生成物。
另外，在专利文献2中，公开了一种蜂窝结构体，其中，蜂窝单元包含无机颗粒、无机纤维以及/或者晶须，无机颗粒是从由氧化铝、二氧化硅、锆、二氧化钛、二氧化铈、莫来石、以及沸石所组成的群中选出的一种以上的无机颗粒。
专利文献1：(日本)特开2006-51499号公报
专利文献2：国际公开第06/137149号小册子
发明内容
本发明想要解决的课题如下：
但是，在专利文献1的方法中存在着这样的问题，即：在SCR系统的下游侧，因为设置了作为另一物体的贵金属触媒，所以SCR系统的配置空间变大了。
另外，目前还存在着一种需求，即：NOx的净化性能要比专利文献2的蜂窝结构体中的无机颗粒为沸石时还高。
本发明是鉴于上述现有技术所具有的问题而提出的，其目的在于提供一种不仅可维持NOx的净化性能还可抑制氨逃逸、并可对SCR系统的配置空间变大进行抑制的蜂窝结构体和尾气净化装置。
用于解决上述课题的手段如下：
一种蜂窝结构体，具有蜂窝单元，在该蜂窝单元中，包含沸石以及无机粘结剂，并且多个贯穿孔隔着间壁沿长度方向并排设置，在所述蜂窝单元中，仅在从所述长度方向的一方的端部起算长度为全长的1.5％以上20％以下的区域内担载贵金属触媒。
所述沸石优选为β型沸石、ZSM-5型沸石、或者磷酸盐系列沸石。
所述磷酸盐系列沸石优选为从SAPO、MeAPO、以及MeAPSO所组成的群中选出的一种以上的沸石。
所述SAPO优选为从SAPO-5、SAPO-11、以及SAPO-34所组成的群中选出的一种以上的SAPO。
所述沸石优选为包含由Cu以及/或者Fe进行了离子交换的沸石。
所述无机粘结剂优选为从氧化铝溶胶、二氧化硅溶胶、二氧化钛溶胶、水玻璃、海泡石、硅镁土、以及伯姆石所组成的群中选出的一种以上的物质中含有的固形成分。
所述蜂窝单元优选为还包含无机纤维以及/或者鳞片状物质。
所述无机纤维优选为从氧化铝、二氧化硅、碳化硅、二氧化硅氧化铝、玻璃、钛酸钾、以及硼酸铝所组成的群中选出的一种以上的无机纤维，所述鳞片状物质优选为从玻璃、白云母、氧化铝、二氧化硅、以及氧化锌所组成的群中选出的一种以上的物质。
本发明的蜂窝结构体优选为具有多个所述蜂窝单元。
本发明的尾气净化装置具有本发明的蜂窝结构体，担载了所述贵金属触媒的区域配置在尾气流动方向的下游侧。
本发明的尾气净化装置优选为使用于柴油发动机的SCR系统。
本发明的效果如下：
根据本发明，能够提供一种不仅可维持NOx的净化性能还可抑制氨逃逸、并可对SCR系统的配置空间变大进行抑制的蜂窝结构体和尾气净化装置。
附图说明
图1是表示本发明的蜂窝结构体的一个例子的立体图。
图2是表示本发明的尾气净化装置的一个例子的截面图。
图3是表示图1的蜂窝结构体的变形例的立体图。
图4是表示用于构成图3的蜂窝结构体的蜂窝单元的立体图。
图5是表示实施例和比较例的评价方法的图。
具体实施方式
下面参考附图对本发明的实施形态进行说明。
图1示出了本发明的蜂窝结构体的一个例子。在蜂窝结构体10中，单一蜂窝单元11的外周面上形成有外周涂层12；该蜂窝单元11包含作为无机颗粒的沸石以及无机粘结剂，并且多个贯穿孔11a隔着间壁11b沿长度方向并排设置。
此时，在蜂窝单元11中，仅在从所述长度方向的一方的端部起算长度为全长的1.5％以上20％以下的区域A内担载贵金属触媒。下面，将担载了贵金属触媒的蜂窝单元11的区域A称为蜂窝单元11的区域A。
如果将这样的蜂窝单元11的区域A配置在尾气净化装置100(参照图2)的尾气流动方向的下游侧，则通过蜂窝单元11的区域A内所担载的贵金属触媒，氨被氧化，这样，就可以抑制氨的逃逸。
这里需要说明的是，尾气净化装置100是在蜂窝结构体10的外周部配置了支撑密封材20的状态下，通过被封装(scanning)至金属管30而得到的。另外，在尾气净化装置100中，在相对于尾气流动方向的蜂窝结构体10的上游侧设置有用于喷射氨或其前躯体的喷射嘴等的喷射单元(图中未示)。据此，氨被添加至尾气中，这样，在蜂窝单元11所含有的沸石上，尾气中所包含的NOx被还原。此时，如果考虑到氨或其前躯体的储藏稳定性，则作为氨的前躯体，优选为使用尿素水。这里需要说明的是，通过在尾气中被加热，尿素水发生水解，产生氨。
如果蜂窝单元11的区域A比从蜂窝单元11的长度方向的一方的端部起算长度为全长的1.5％的区域还小，则对氨逃逸进行抑制的效果不足。而如果蜂窝单元11的区域A比从蜂窝单元11的长度方向的一方的端部起算长度为全长的20％的区域还大，则NOx的净化率下降。
作为在蜂窝单元11中被担载的贵金属触媒，只要其可对氨进行氧化，对其并无特别限定，可列举出铂(白金)、钯、铑等，也可以同时使用其中的两种以上的贵金属触媒。
作为在蜂窝单元11中所包含的沸石，对其并无特别限定，可列举出β型沸石、ZSM-5型沸石、磷酸盐系列沸石等，也可以同时使用其中的两种以上的沸石。其中，为了提高NOx的净化性能，优选为磷酸盐系列沸石。
作为磷酸盐系列沸石，可列举出SAPO-5、SAPO-11、SAPO-34等的SAPO；MeAPO；MeAPSO等。
如果考虑到NOx的净化能力，沸石优选为包含由Cu以及/或者Fe进行了离子交换的沸石。这里需要说明的是，沸石还可以包含没有被离子交换的沸石、以及由上述金属以外的金属进行了离子交换的沸石。
由Cu以及/或者Fe进行了离子交换的沸石的离子交换量优选为1.0～5.0质量％。如果离子交换量小于1.0质量％，则NOx的净化性能有可能不足，而如果大于5.0质量％，则应该被离子交换的金属可能作为氧化物而存在，导致有可能不能被离子交换。
另外，沸石的一次颗粒或二次颗粒的平均粒径优选为0.5～10μm，最好为1～5μm。如果沸石的一次颗粒或二次颗粒的平均粒径小于0.5μm，则尾气难以渗透至间壁11b的内部，沸石有可能不能有效地用于NOx的净化。而如果沸石的一次颗粒或二次颗粒的平均粒径大于10μm，则因为蜂窝单元11中的气孔数量变少，所以尾气难以渗透至间壁11b的内部，导致沸石有可能不能有效地用于NOx的净化。
蜂窝单元11的单位表观体积的沸石含量优选为230～360g/L。如果单位表观体积的沸石含量小于230g/L，则为了提高NOx的净化率，有可能一定要增大蜂窝单元11的表观体积。而如果单位表观体积的沸石含量大于360g/L，则蜂窝单元11的强度有可能不足、或者蜂窝单元11的开口率有可能变小。
作为包含在蜂窝单元11内的无机粘结剂，对其并无特别限定，可列举出氧化铝溶胶、二氧化硅溶胶、二氧化钛溶胶、水玻璃、海泡石、硅镁土、伯姆石等所含有的固形成分，也可以同时使用其中的两种以上的无机粘结剂。
蜂窝单元11的无机粘结剂的含量优选为5～30质量％，最好为10～20质量％。如果无机粘结剂的含量小于5质量％，则蜂窝单元11的强度有可能下降，而如果大于30质量％，则有可能难以进行蜂窝单元11的挤压成型。
为了提高强度，蜂窝单元11优选为还包含无机纤维以及/或者鳞片状物质。
作为包含在蜂窝单元11内的无机纤维，只要其可以提高蜂窝单元11的强度，对其并无特别限定，可列举出氧化铝、二氧化硅、碳化硅、二氧化硅氧化铝、玻璃、钛酸钾、硼酸铝等，也可以同时使用其中的两种以上的无机纤维。
无机纤维的纵横比优选为2～1000，较好为5～800，最好为10～500。如果无机纤维的纵横比小于2，则对蜂窝单元11的强度进行提高的效果有可能变小。而如果无机纤维的纵横比大于1000，则对蜂窝单元11进行挤压成型时，在模具内有可能发生网眼堵塞等情况，还有可能由于无机纤维发生折断，导致对蜂窝单元11的强度进行提高的效果变小。
作为包含在蜂窝单元11内的鳞片状物质，只要其可以提高蜂窝单元11的强度，对其并无特别限定，可列举出玻璃、白云母、氧化铝、二氧化硅、氧化锌等，也可以同时使用其中的两种以上的鳞片状物质。蜂窝单元11的无机纤维以及鳞片状物质的含量优选为3～50质量％，较好为3～30质量％，最好为5～20质量％。如果无机纤维以及鳞片状物质的含量小于3质量％，则对蜂窝单元11的强度进行提高的效果有可能变小。而如果无机纤维以及鳞片状物质的含量大于50质量％，则蜂窝单元11中的沸石含量降低，导致NOx的净化率有可能下降。蜂窝单元11的气孔率优选为25～40％。如果蜂窝单元11的气孔率小于25％，则尾气难以渗透至间壁11b的内部，沸石就可能不能有效地用于NOx的净化。而如果蜂窝单元11的气孔率大于40％，则蜂窝单元11的强度有可能不足。
这里需要说明的是，蜂窝单元11的气孔率可使用水银压入法来进行测定。
蜂窝单元11的与长度方向垂直的截面的开口率优选为50～75％。如果与长度方向垂直的截面的开口率小于50％，则沸石有可能不能有效地用于NOx的净化。而如果与长度方向垂直的截面的开口率大于75％，则蜂窝单元11的强度有可能不足。
蜂窝单元11的与长度方向垂直的截面的贯穿孔11a的密度优选为31～124个/cm2。如果与长度方向垂直的截面的贯穿孔11a的密度小于31个/cm2，则废气与沸石难以发生接触，NOx的净化率有可能下降。而如果与长度方向垂直的截面的贯穿孔11a的密度大于124个/cm2，则蜂窝结构体10的压力损失可能增大。
蜂窝单元11的间壁11b的厚度优选为0.10～0.50mm，最好为0.15～0.35mm。如果间壁11b的厚度小于0.10mm，则蜂窝单元11的强度有可能降低。而如果间壁11b的厚度大于0.50mm，则废气难以渗透至间壁11b的内部，导致沸石有可能不能有效地用于NOx的净化。
外周涂层12的厚度优选为0.1～2mm。如果外周涂层12的厚度小于0.1mm，则对蜂窝结构体10的强度进行提高的效果有可能不足。而如果外周涂层12的厚度大于2mm，则蜂窝结构体10的单位体积的沸石含量降低，导致NOx的净化率有可能下降。
蜂窝结构体10为圆柱状，但并不限定于此，也可为棱柱状、椭圆柱状等。另外，贯穿孔11a的形状为四棱柱状，但并不限定于此，也可为三棱柱状、六棱柱状等。
下面，对蜂窝结构体10的制造方法的一个例子进行说明。首先，使用原料膏进行挤压成型，以制成多个贯穿孔隔着间壁沿长度方向并排设置的圆柱状蜂窝成型体毛坯，其中，该原料膏包含沸石以及无机粘结剂，另外，根据需要，还可包含无机纤维以及/或者鳞片状物质。据此，即使将烧成温度设为较低，也可以得到具有足够强度的圆柱状蜂窝单元11。
这里需要说明的是，作为原料膏中所包含的无机粘结剂，可添加氧化铝溶胶、二氧化硅溶胶、二氧化钛溶胶、水玻璃、海泡石、硅镁土、伯姆石等，也可以同时使用其中的两种以上的无机粘结剂。
另外，根据需要，在原料膏中还可以适当地添加有机粘结剂、分散介质、成型辅助剂等。
作为有机粘结剂，对其并无特别限定，可列举出甲基纤维素、羧甲基纤维素、羟乙基纤维素、聚乙二醇、酚醛树脂、环氧树脂等，也可以同时使用其中的两种以上的有机粘结剂。这里需要说明的是，有机粘结剂的添加量优选为沸石、无机粘结剂、无机纤维、以及鳞片状物质的总质量的1～10％。
作为分散介质，对其并无特别限定，可列举出水、苯等的有机溶液、甲醇等醇等，也可以同时使用其中的两种以上的分散介质。
作为成型辅助剂，对其并无特别限制，可列举出乙二醇、糊精、脂肪酸、脂肪酸肥皂、多元醇等，也可以同时使用其中的两种以上的成型辅助剂。
调制原料膏时，优选为进行混合混炼，可以使用搅拌器、磨碎机等进行混合，也可以使用捏合机等进行混炼。
然后，使用微波干燥机、热风干燥机、电感(高频)干燥机、减压干燥机、真空干燥机、冻结干燥机等干燥机对所得到的蜂窝成型体进行干燥。
接下来，对所得到的蜂窝成型体进行脱脂。对脱脂条件并无特别限定，其可以根据成型体内所包含的有机物的种类和含量进行适当的选择，优选为在400℃下脱脂2个小时。
之后，通过对所得到的蜂窝成型体进行烧成，得到圆柱状蜂窝单元11。烧成温度优选为600～1200℃，最好为600～1000℃。如果烧成温度小于600℃，则烧结不进行，蜂窝单元11的强度有可能变低。而如果烧成温度大于1200℃，则烧结过度进行，沸石的反应部位有可能减少。
接下来，在圆柱状蜂窝单元11的外周面上涂敷外周涂层用膏。
作为外周涂层用膏，对其并无特别限制，可列举出无机粘结剂和无机颗粒的混合物、无机粘结剂和无机纤维的混合物、无机粘结剂、无机颗粒和无机纤维的混合物等。
另外，外周涂层用膏还可以包含有机粘结剂。作为有机粘结剂，对其并无限定，可列举出聚乙烯醇、甲基纤维素、乙基纤维素、羧甲基纤维素等，也可以同时使用其中的两种以上的有机粘结剂。
然后，通过对涂敷了外周涂层用膏的蜂窝单元11进行干燥固化，得到圆柱状蜂窝结构体10。此时，如果外周涂层用膏内包含了有机粘结剂，则优选为进行脱脂。脱脂条件可以根据有机物的种类和含量进行适当的选择，优选为在700℃下脱脂20分钟。
这里需要说明的是，通过将蜂窝单元11浸渍在含有Cu离子或Fe离子的水溶液中，可以对沸石进行离子交换。另外，也可以使用包含由Cu以及/或者Fe离子进行了离子交换的沸石的原料膏。
另外，使用含浸法(浸渍法)，可以使蜂窝单元11的区域A担载贵金属触媒。此时，也可以使蜂窝单元11的区域A担载氧化铝等的载体，该载体上担载了贵金属触媒。另外，使蜂窝单元11的区域A担载氧化铝等的载体后，还可以使其担载贵金属触媒。再有，也可以使蜂窝单元11的区域A直接担载贵金属触媒。
图3示出了蜂窝结构体10的变形例。这里需要说明的是，在蜂窝结构体10’中，多个蜂窝单元11通过粘结层13被粘结在一起，其中，在每个蜂窝单元11中，多个贯穿孔11a隔着间壁11b沿长度方向并排设置(参照图4)；除此之外，蜂窝结构体10’与蜂窝结构体10相同。
蜂窝单元11的与长度方向垂直的截面的截面面积优选为5～50cm2。如果与长度方向垂直的截面的截面面积小于5cm2，则蜂窝结构体10’的压力损失有可能增大。而如果与长度方向垂直的截面的截面面积大于50cm2，则相对于蜂窝单元11内所产生的热应力的强度有可能不足。
粘结层13的厚度优选为0.5～2mm。如果粘结层13的厚度小于0.5mm，则粘结强度有可能不足。而如果粘结层13的厚度大于2mm，则蜂窝结构体10’的压力损失有可能增大。
另外，周缘部之外的蜂窝单元11的形状为四棱柱状，但对其并无特别限定，例如也可为六棱柱等。
下面，对蜂窝结构体10’的制造方法的一个例子进行说明。首先，与蜂窝结构体10同样地制成四棱柱状蜂窝单元11。接下来，在蜂窝单元11的外周面上涂敷粘结层用膏，然后按顺序使蜂窝单元11粘结，并进行干燥固化，以制成蜂窝单元11的集合体。
此时，在制成蜂窝单元11的集合体后，也可以将其切削成圆柱状，并进行研磨。另外，也可以使截面被形成为扇形或正方形的蜂窝单元11进行粘结，以制成圆柱状蜂窝单元11的集合体。
作为粘结层用膏，对其并无特别限定，可列举出无机粘结剂和无机颗粒的混合物、无机粘结剂和无机纤维的混合物、无机粘结剂、无机颗粒和无机纤维的混合物等。
另外，粘结层用膏还可以包含有机粘结剂。作为有机粘结剂，对其并无特别限定，可列举出聚乙烯醇、甲基纤维素、乙基纤维素、羧甲基纤维素等，也可以同时使用其中的两种以上的有机粘结剂。
接下来，在圆柱状蜂窝单元11的集合体的外周面上涂敷外周涂层用膏。对外周涂层用膏并无特别限定，其可以包含与粘结层用膏相同的材料，也可以包含不同的材料。另外，外周涂层用膏还可以与粘结层用膏具有相同的组成。
之后，通过对涂敷了外周涂层用膏的蜂窝单元11的集合体进行干燥固化，得到圆柱状蜂窝结构体10’。此时，如果粘结层用膏以及/或者外周涂层用膏内包含了有机粘结剂，则优选为进行脱脂。脱脂条件可以根据有机物的种类和含量进行适当的选择，优选为在700℃下脱脂20分钟。
这里需要说明的是，在蜂窝结构体10以及10’中，也可以不形成外周涂层12。
[实施例1]
首先，将平均粒径为3μm的SAPO 3100g、伯姆石895g、平均纤维直径为6μm且平均纤维长度为100μm的氧化铝纤维485g、甲基纤维素380g、油脂酸(olein acid)280g、以及离子交换水2425g进行混合混炼，以制成原料膏1。
然后，使用挤压成型机对原料膏1进行挤压成型，制成正四棱柱状的蜂窝成型体毛坯。接下来，使用微波干燥机以及热风干燥机，在110℃下对蜂窝成型体进行10分钟的干燥处理，之后，在400℃下实施5个小时的脱脂。接下来，在700℃下进行2个小时的烧成，制成边长为34.3mm、长度为150mm的正四棱状蜂窝单元11。在蜂窝单元11中，贯穿孔11a的密度为93个/cm2，间壁11b的厚度为0.23mm。
之后，通过将蜂窝单元11浸渍在硝酸铜水溶液中，由Cu离子对沸石进行了交换。使用ICPS-8100(“岛津制作所”公司制)通过IPC发光分析所求得的沸石的离子交换量为2.7质量％。
另外，将蜂窝单元11的区域A(长度为10mm)浸渍在硝酸白金溶液中后，在600℃下保持1个小时，使其担载白金触媒。此时，蜂窝单元11的区域A的单位表观体积的白金触媒含量为3g/L。
接下来，将平均纤维直径为0.5μm且平均纤维长度为15μm的氧化铝纤维767g、石英玻璃2500g、羧甲基纤维素17g、固形成分为30质量％的二氧化硅溶胶600g、聚乙烯醇167g、界面活性剂167g、以及氧化铝中空球(alumina balloon)17g进行混合混炼，以制成具有耐热性的粘结层用膏。
涂敷粘结层用膏，以使粘结层的厚度为2mm，然后，使16个蜂窝单元11进行粘结，并对粘结层用膏在150℃下进行10分钟的干燥固化，之后，使用钻石切割器将其切削成与长度方向垂直的截面大致为点对称的圆柱状，以制成蜂窝单元11的集合体。
接下来，在蜂窝单元11的集合体的外周面上涂敷粘结层用膏，以使外周涂层的厚度为1mm，之后，使用微波干燥机和热风干燥机，在150℃下对粘结层用膏进行10分钟的干燥固化，然后，在400℃下实施2个小时的脱脂，以制成直径为143.8mm、高度为150mm的圆柱状蜂窝结构体10’。
之后，在于蜂窝结构体10’的外周部配置了支撑密封材(由无机纤维构成的垫材)20的状态下，将其封装入金属管(外壳)30，以制成尾气净化装置100’(参照图2)。此时，蜂窝单元11的区域A被配置在相对于尾气流动方向的下游侧。
[实施例2]
除了将蜂窝单元11的区域A的长度变更为5mm之外，与实施例1同样地制成蜂窝结构体10’和尾气净化装置100’。
[实施例3]
除了将蜂窝单元11的区域A的长度变更为25mm之外，与实施例1同样地制成蜂窝结构体10’和尾气净化装置100’。
[实施例4]
将平均粒径为3μm的β型沸石3000g、伯姆石840g、平均纤维直径为6μm且平均纤维长度为100μm的氧化铝纤维650g、甲基纤维素330g、油脂酸(olein acid)330g、以及离子交换水1800g进行混合混炼，以制成原料膏2。
除了以原料膏2代替原料膏1之外，与实施例2同样地制成蜂窝结构体10’和尾气净化装置100’。
[实施例5]
除了通过将蜂窝单元11浸渍至硝酸铁水溶液中，由Fe离子对沸石进行离子交换之外，与实施例4同样地制成蜂窝结构体10’以及尾气净化装置100’。
这里需要说明的是，使用ICPS-8100(“岛津制作所”公司制)通过IPC发光分析所求得的沸石的离子交换量为2.7质量％。
[实施例6]
除了将蜂窝单元11的区域A的长度变更为25mm之外，与实施例5同样地制成蜂窝结构体10’以及尾气净化装置100’。
[实施例7]
将由Cu进行了2.7质量％离子交换且平均粒径为3μm的SAPO3100g、伯姆石895g、平均纤维直径为6μm且平均纤维长度为100μm的氧化铝纤维485g、甲基纤维素380g、油脂酸(olein acid)280g、以及离子交换水2425g进行混合混炼，以制成原料膏3。
除了以原料膏3代替原料膏1，并且不将蜂窝单元11浸渍至硝酸铜水溶液之外，与实施例2同样地制成蜂窝结构体10’和尾气净化装置100’。
[实施例8]
将由Fe进行了2.7质量％离子交换且平均粒径为3μm的β型沸石3000g、伯姆石840g、平均纤维直径为6μm且平均纤维长度为100μm的氧化铝纤维650g、甲基纤维素330g、油脂酸(olein acid)330g、以及离子交换水1800g进行混合混炼，以制成原料膏4。
除了以原料膏4代替原料膏1，并且不将蜂窝单元11浸渍至硝酸铜水溶液之外，与实施例2同样地制成蜂窝结构体10’和尾气净化装置100’。
[比较例1]
除了将蜂窝单元11的区域A的长度变更为2mm之外，与实施例1同样地制成蜂窝结构体10’以及尾气净化装置100’。
[比较例2]
除了在蜂窝单元11上不担载白金触媒之外，与实施例1同样地制成蜂窝结构体10’以及尾气净化装置100’。
[比较例3]
除了将蜂窝单元11的区域A的长度变更为2mm之外，与实施例5同样地制成蜂窝结构体10’以及尾气净化装置100’。
[比较例4]
除了在蜂窝单元11上不担载白金触媒之外，与实施例5同样地制成蜂窝结构体10’以及尾气净化装置100’。
[比较例5]
除了在蜂窝单元11上不担载白金触媒之外，与实施例7同样地制成蜂窝结构体10’以及尾气净化装置100’。
[比较例6]
除了在蜂窝单元11上不担载白金触媒之外，与实施例8同样地制成蜂窝结构体10’以及尾气净化装置100’。
[NOx净化率的测定以及氨逃逸的评价]
如图5所示，在经由排气管将柴油发动机(1.6L直喷引擎)200、柴油氧化触媒(DOC)300、柴油颗粒捕集(过滤)器(DPF)400、实施例1～8以及比较例1～6的各尾气净化装置100’进行串联连接的状态下，在NEDC(New European Driving Cycle)模式下使其运转。此时，使用MEXA-7500DEGR(“HORIBA”公司制)，对流入尾气净化装置100’的NOx流入量以及从尾气净化装置100’流出的NOx流出量进行测定，并对由下式所表示的NOx净化率[％]进行了测定(检测界限为0.1ppm)。
(NOx流入量-NOx流出量)/(NOx流入量)×100
此时，在尾气净化装置100’之前的紧挨着的排气管中，一边对从柴油发动机200排出的NOx进行检测，一边喷射尿素水，以使尿素相对于NOx的摩尔比为1.2。这里需要说明的是，尾气净化装置100’的平均温度为160℃，平均空间速度(SV)为20000/hr，尾气中二氧化氮相对于NOx的体积比为0.25～0.30，仅在尾气净化装置100’的温度为180℃以上时喷射尿素水，使尾气净化装置100’的蜂窝结构体10’预先吸收6.0g的氨。
另外，在尾气净化装置100’的下游侧设置气体检测管，以对是否存在氨逃逸进行评价。
此时，作为DOC 300以及DPF 400，分别使用直径为143.8mm且长度为100mm的蜂窝结构体(商品)、以及直径为143.8mm且长度为152.4mm的蜂窝结构体(商品)。
这里需要说明的是，在使用比较例2、4的尾气净化装置100’的情况下，在图5中，于尾气净化装置100’的下游侧，经由排气管，还设置作为DOC的直径为143.8mm且长度为50mm的蜂窝结构体(商品)。
表1中示出了NOx净化率的测定结果以及氨逃逸的评价结果。
[表1]
Figure BPA00001562603400151
Figure BPA00001562603400161
由表1可知，实施例1～8的尾气净化装置100’不仅可以维持NOx净化率，而且还可以抑制氨逃逸。此时，如果在比较例2、4的尾气净化装置100’的下游侧经由排气管另外设置DOC，则也可以抑制氨逃逸。但是，如果在比较例2、4的尾气净化装置100’的下游侧不设置经由排气管的DOC，则不能抑制氨逃逸。另外还可知，在实施例1～8的尾气净化装置100’的下游侧，可以不设置经由排气管的DOC，所以，实施例1～8的尾气净化装置100’可以对SCR系统的配置空间的变大进行抑制。
因此可知，通过仅在蜂窝元11的相对于长度方向的、从一个端部开始的全长的1.5～20％的区域A内担载贵金属触媒，蜂窝结构体10’以及尾气净化装置100’不仅可以维持NOx净化性能，还可以抑制氨逃逸，另外，还可以对SCR系统的配置空间的变大进行抑制。
这里需要说明的是，在本实施例中，尽管示出了蜂窝结构体10’，但是，可以认为，对蜂窝结构体10而言，也可以得到相同的效果。
符号说明
10、10’ 蜂窝结构体
11 蜂窝单元
11a 贯穿孔
11b 间壁
A 第一区域
B 第二区域
12 外周涂层
13 粘结层
20 支撑密封材
30 金属管
100、100’ 尾气净化装置

Claims (9)

1.一种尾气净化装置，其使用于柴油发动机的SCR系统，该尾气净化装置使用蜂窝结构体，其特征在于，
所使用的蜂窝结构体具有蜂窝单元，该蜂窝单元为使用包含沸石以及无机粘结剂的原料膏进行挤压成型而沿长度方向隔着间壁并排设置有多个贯穿孔的蜂窝单元，
在所述蜂窝单元中，仅在从所述长度方向的一方的端部起算长度为全长的1.5％以上20％以下的区域内担载贵金属触媒，
所述蜂窝单元的担载了所述贵金属触媒的区域配置在尾气流动方向的下游侧，
贵金属触媒对氨进行氧化。
2.根据权利要求1所述的尾气净化装置，其特征在于，
所述沸石为β型沸石、ZSM-5型沸石、或者磷酸盐系列沸石。
3.根据权利要求2所述的尾气净化装置，其特征在于，
所述磷酸盐系列沸石为从SAPO、MeAPO、以及MeAPSO所组成的群中选出的一种以上的沸石。
4.根据权利要求3所述的尾气净化装置，其特征在于，
所述SAPO为从SAPO-5、SAPO-11、以及SAPO-34所组成的群中选出的一种以上的SAPO。
5.根据权利要求1至4的任1项所述的尾气净化装置，其特征在于，
所述沸石为包含由Cu以及／或者Fe进行了离子交换的沸石。
6.根据权利要求1至4的任1项所述的尾气净化装置，其特征在于，
所述无机粘结剂为从氧化铝溶胶、二氧化硅溶胶、二氧化钛溶胶、水玻璃、海泡石、硅镁土、以及伯姆石所组成的群中选出的一种以上的物质中含有的固形成分。
7.根据权利要求1至4的任1项所述的尾气净化装置，其特征在于，
所述蜂窝单元还包含无机纤维以及／或者鳞片状物质。
8.根据权利要求7所述的尾气净化装置，其特征在于，
所述无机纤维为从氧化铝、二氧化硅、碳化硅、二氧化硅氧化铝、玻璃、钛酸钾、以及硼酸铝所组成的群中选出的一种以上的无机纤维，
所述鳞片状物质为从玻璃、白云母、氧化铝、二氧化硅、以及氧化锌所组成的群中选出的一种以上的物质。
9.根据权利要求1至4的任1项所述的尾气净化装置，其特征在于，
具有多个所述蜂窝单元。
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