CN1777740B - 用于处理内燃机废气的多孔片和具有多孔片的基板 - Google Patents

用于处理内燃机废气的多孔片和具有多孔片的基板 Download PDF

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CN1777740B
CN1777740B CN2004800103534A CN200480010353A CN1777740B CN 1777740 B CN1777740 B CN 1777740B CN 2004800103534 A CN2004800103534 A CN 2004800103534A CN 200480010353 A CN200480010353 A CN 200480010353A CN 1777740 B CN1777740 B CN 1777740B
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supporter
mesh sheet
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sheet
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CN1777740A (zh
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奥利斯·瓦基莱宁
雷约·吕吕坎加斯
里特瓦·海基宁
图沃·毛努拉
马蒂·海尔克宁
阿里·列沃宁
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Abstract

本发明的目的是一种用于在畅通通道中处理内燃机的废气的多孔片。根据本发明，多孔片(3，3a，3b)的至少一部分具有覆盖支撑物(33)，所述覆盖支撑物(33)具有超过10nm的小孔(35)以及超过1.4μm的粗颗粒。

Description

用于处理内燃机废气的多孔片和具有多孔片的基板 
技术领域
本发明涉及一种用于在畅通通道中处理内燃机废气的多孔片以及具有所述多孔片的基板。本发明还涉及用于制造所述多孔片以及具有所述多孔片的基板的方法。 
背景技术
为了处理内燃机的废气，需要使用具有畅通或闭合通道或者两者结合的基板。在畅通通道中废气直接流过基板。在具有闭合通道的基板中，废气被强迫流过壁，例如陶瓷或金属多孔壁。在畅通通道中气态杂质的减少通常较高，但杂质颗粒的减少较低，例如只有10％到15％。在闭合通道中气态杂质的减少较高，且杂质颗粒的减少也较高，例如70％到90％。闭合通道中的问题是壁的堵塞。如果闭合通道没有被清理的话，它将逐渐完全堵塞。压力损失也会增加。一种保持通道畅通的方法是不断或定时清理它们。 
一种困难的情形是使用部分堵塞的具有闭合通道的基板起动内燃机。所述基板的温度在起动时较低，颗粒被捕捉在表面上。最终壁面上有太多颗粒以至于阻止废气的流动。这种情况下甚至可能损害内燃机。 
WO 03038248 A1(2003年5月8日公开)批露了一种过滤复合介质，由此流体能流过该过滤复合介质。该过滤复合介质包括至少一 个顶层，其由带有至少一个边缘区域的至少部分地多孔材料制成，该过滤复合介质包括由纤维布制成的至少一个纤维层。过滤复合介质的特征在于：至少一个纤维层形成围壁，其围住纤维层使得纤维层永久地设在所述的至少一个顶层内。 
发明内容
现在已经发明了一种多孔片，其在畅通通道中有效地减少废气中的颗粒。相应地还发明了一种具有所述多孔片的基板。 
为此，本发明的特征在于独立权利要求中描述的事实。其它权利要求批露了本发明的一些优选实施例。 
可以故意使本发明的片的表面粗糙，从而促进物质和热量传递和/或颗粒去除/反应。粗糙度可以例如用诸如30-100μm的纤维的粗糙原材料和/或涂覆方法提供。粗糙度、支撑物厚度和/或催化活性层的数量优选地沿一个或更多个催化剂的轴向变化。 
本发明的构造实施例没有任何特别限制。根据本发明的实施例，本发明的催化剂可以呈现相对于流动方向平行或串联的几种结构。 
根据本发明的实施例，多孔片至少部分地被具有超过10nm的小孔以及超过1.4μm的粗颗粒的支撑物覆盖。优选地，基本上多孔片的所有小孔都填充有所述支撑物。优选地，所述多孔片存在两种尺寸的畅通通道。不必使用例如纤维层的额外的层作为支撑物和/或过滤装置。被涂覆的多孔片的结构简单，它们易于制造，并且与用在畅通通道中的平滑片相比颗粒的减少较高。 
意外地发现当用具有超过10nm的小孔以及超过1.4μm的粗颗粒的支撑物覆盖多孔片时，在畅通通道中流动的颗粒的减少显著提 高。颗粒的减少非常依赖于颗粒源和颗粒组分。颗粒能包括不同量的挥发性有机化合物(VOF’s)、固态碳、硫磺、水和金属氧化物。标准氧化催化剂能氧化大部分VOF’s并这样减少10％到60％的颗粒物质。利用本发明可以将颗粒减少提高20％到25％。 
新型多孔片的重要特征在于它根本不会堵塞或者堵塞最小。这非常重要，依据本发明的多孔片能用在大多数要求很高的环境中，它们可用于很多场合。 
畅通通道中气体流动由于支撑物的小孔和粗颗粒而在多孔片的表面被降低。涂覆有具有小孔和粗颗粒的材料的多孔片起畅通的颗粒捕捉器的作用。这样增加了杂质气体和颗粒的接触，从而增加保持时间和并促进杂质减少。与平滑片相比，杂质颗粒更经常地附着到多孔片。 
附着到多孔片的颗粒分解成气态杂质，该气态杂质进一步分解成无害化合物。一部分气体在多孔片的开口中流过支撑物的小孔，颗粒附着到支撑物的表面上。这也能更好地减少颗粒。另一方面，多孔片不会堵塞，或者堵塞最小，在多孔片附近压力损失以及气体的流量不会降低。这样减少了操作中的失败，从而提高多孔片的效率。 
多孔片两侧的压差促进废气流过多孔片和支撑物的小孔。这种现象导致颗粒附着到支撑物上，并更好地减少废气中的颗粒。 
根据本发明的实施例，所述支撑物的中值孔尺寸超过5nm，优选地10到50nm，例如15到20nm。支撑物的最佳孔尺寸取决于废气以及多孔片附近气体流动的环境。废气可以具有例如5到200nm的中值颗粒尺寸而中值孔尺寸可以为5到20nm。 
多孔片可以优选地是网状片或金属泡沫片、烧结金属片、经编金 属丝网、陶瓷纤维片等。根据本发明的实施例，多孔片为网状片。优选地，网状片的网目数为30到300。至少一部分废气能在网状片的开口中流过具有超过10nm的小孔的支撑物。这样导致废气中的颗粒附着到支撑物的表面，从而更好地减少颗粒。 
根据本发明的实施例，网状片的中值开口尺寸为0.01到0.5nm，优选地为0.05到0.3nm，例如0.08到0.2nm。 
多孔片的开口的形状也可以不同。它可以是沟渠状、正方形、菱形或孔状。例如，在菱形网状片中，金属丝可以处于一个层面或者它们相互交叉。 
多孔片可以是例如波纹的或平直的。优选地，所述多孔片是波纹片，诸如波纹网状片。这样增加杂质气体和颗粒与支撑物的接触，从而增加保持时间并促进杂质的减少。 
根据本发明的实施例，所述支撑物包括纤维，该纤维从所述支撑物的平面突出来。这样还通过降低颗粒的流速从而促进颗粒附着到支撑物上来减少颗粒。 
粗糙支撑物可以通过例如碾磨制造。将粗颗粒组分加入到碾磨过程显著改变了支撑物的孔尺寸分布。粗糙支撑物材料可以通过球磨机将载体涂层浆和粗氧化铝颗粒碾磨在一起30到120分钟，例如40到60分钟而制得。 
根据本发明的实施例，支撑物的中值颗粒尺寸超过1μm，优选地1.4到15μm，例如2到10μm。该值部分地取决于废气的中值颗粒尺寸以及多孔片表面附近气体的流速。它还取决于多孔片的孔尺寸。粗支撑物的表面质量可以是例如20到200g/m2，优选地20到80g/m2，例如35到50g/m2。通过BET方法测得的支撑物的比表面积可 以是例如30到300m2/g，优选地150到250m2/g，例如150到200m2/g。 
粗颗粒可以是，例如氧化铝、氧化硅、氧化锆、氧化铈或/和氧化钛颗粒。也能使用适合于废气处理的其它颗粒。最适合的颗粒是例如粗氧化铝颗粒，其可以很容易地被球磨机碾磨。这些所选的氧化铝颗粒和最初一样是圆形形状，因而通过碾磨可以维持对气体净化的适当效果。最初的中值颗粒尺寸可以是100到200μm，优选地150到200μm，例如170μm。 
根据本发明的实施例，支撑物包括催化惰性粗氧化铝、氧化硅、氧化锆、氧化铈或/和氧化钛颗粒。优选地，至少一部分支撑物是通过将催化活性细支撑物材料和催化非活性粗颗粒在一起碾磨制得。优选的所述支撑物包括易于碾磨的粗材料。 
根据本发明的实施例，孔隙体积优选地为0.3到0.8cm3/g，例如0.4cm3/g。 
根据本发明的实施例，所述支撑物包括催化活性细材料。 
根据本发明的实施例，所述支撑物包括催化惰性粗材料。 
为氧化目的而制备的催化剂载体涂层是最合适的。尽管任何载体涂层都可以通过所选粗颗粒而变粗糙。典型的氧化载体涂层和图8中显示的一样。BET比表面积可以是例如230m2/g，中值颗粒尺寸可以是例如1.5到3.5μm，支撑物的面积质量可以是例如40g/m2。 
根据本发明的实施例，具有畅通通道的基板包括至少一个根据本发明的多孔片。优选地，所述片为波纹片。更优选地所述片为波纹网状片。具有所述多孔片的基板起畅通的颗粒捕捉器的作用，这样促进颗粒的减少。另一方面，基板的畅通通道不会堵塞，或者堵塞最小，基板中的压力损失以及气体的流速也不会降低。这样减少操作中的失 败，从而提高基板的效率。 
所述基板还能包括除了根据本发明的多孔片之外的其它的片。其它的片可以是例如，平直的、波纹的、平滑的、穿孔的、网状片，金属丝网状片或纤维片。 
根据本发明的实施例，其它的片是波纹片。优选地，所述其它的片是波纹网状片。通过使用波纹网状片作为其它的片增加了颗粒的保持时间，也增加了颗粒的碰撞。这些都促进颗粒减少，因而提高基板的效率。 
根据本发明的实施例，其它的片是金属丝网状片，通过在基板中使用金属丝网状片，通过增加颗粒在所述基板中的保持时间能改善颗粒的减少。 
根据本发明的实施例，其它的片是纤维片，通过在基板中使用纤维片，可以通过增加颗粒在所述基板中的保持时间来促进颗粒减少。 
根据本发明的实施例，其它的片已经至少部分地被支撑物覆盖。该支撑物可以是与用于多孔片相同的支撑物，或者也可以是不同的支撑物。由于其它的片的优选支撑物包括粗颗粒和/或纤维，其从所述支撑物的平面突出来。优选地，其它的片上的支撑物具有超过0.4μm，例如1.5到3.5μm的中值颗粒尺寸。这实质上促进颗粒的附着，因而促进颗粒在所述基板中减少。 
根据本发明的实施例，其它的片基本上被具有超过1.4μm的中值颗粒尺寸和/或具有超过10nm的小孔的支撑物覆盖。这样也通过促进颗粒附着到片而促进杂质颗粒的减少。 
根据本发明的实施例，多孔片和/或其它的片具有压痕和/或突起。这增加了气体以及杂质到基板表面的碰撞，从而促进颗粒的减少。这样导致更好的废气中杂质颗粒的减少值。气体的碰撞还导致气体与催化活性材料更好的接触，从而促进气态杂质的减少。 
内燃机废气中的颗粒可以用具有根据本发明的多孔片的基板有效地处理。与传统基板相比，杂质颗粒的减少非常高。另外气态杂质的减少也很高。根据本发明的多孔片不会堵塞或者堵塞最小，使得它不会影响基板中废气的流速。此外基板中的压力损失也最小。 
基板可以是例如预-氧化催化剂或SCR-催化剂。它也可以是水解催化剂。基板可以优选地用于净化内燃机的废气中的杂质颗粒。基板的结构也可以变化。它可以是例如圆形或层叠状。 
根据本发明的实施例，催化剂可以涂覆在一个或多个催化基板上，该催化基板由金属、陶瓷、金属氧化物、SiC和/或Si的氮化物材料制造。本发明的催化剂涂层可以预先或在后涂覆在正常的陶瓷或金属胞或基板上，其中胞的形状可以是正方形或三角形，胞密度(10-2000cpsi，每平方英寸胞数，现有技术中普通技术人员熟知的术语)或壁厚(10-500μm)也可以根据应用广泛地变化。如果废气含有大量颗粒或硫化物，则非常大的通道尺寸可以用在催化剂中(＜100cpsi)。在含有少量颗粒和硫磺的应用中，非常小的通道尺寸可以用在胞中(例如＞500cpsi)。在柴油机应用中，典型的胞数为50到600cpsi。这些变量的值也可以在胞内或在下一些胞中变化，由于有效混合、低压降或机械强度这是优选的。 
要涂覆的胞还在分离通道中用作一种具有混合区域的静态混合结构(例如横向构架、流动障碍、或节流器)，或者通过按下述方式层叠波纹、曲面箔或片而制成的结构：其中波峰的方向偏离进气的方向，层叠的片的波峰分别朝向不同方向。在常规金属胞中，波纹箔的波峰彼此平行，与主流方向平行。 
根据本发明的实施例，基板涂覆有一个或多个胞状或多孔结构。其通道可以平行于流动方向并且/或具有不同朝向。根据本发明的另一实施例，基板涂覆有一个或多个颗粒分离和/或混合结构。根据本发明的实施例，基板结合有颗粒捕捉器、或由陶瓷、金属、金属氧化物、SiO2、SiC和/或Si的氮化物材料制成的过滤器。 
混合效率可以通过改变波纹与主流方向之间的角度来控制。利用混合结构，可以沿管的径向提供流动混合。利用混合结构，可以获得与正常胞结构相比更高的颗粒分离速率。此外，要涂覆的结构可以部分地或完全由金属丝网、烧结多孔金属、纤维、或颗粒捕捉器构成。 
本发明的催化剂还可以涂覆有于平行于流动方向或串联的两种或多种上述催化剂结构。不同的或者相同尺寸的催化剂结构可以被包括在单个催化剂转换器中，或者它们也可以在通过必要管道相互连接的分离的转换器中。本发明的催化剂的组分、其贵金属装载量(load)(例如Pt)、胞数(几何表面积)、或结构可以相同或不同。 
最新的柴油机通常设有涡轮，因此排气管中的温度较低，没有非常靠近发动机的空间用于大的转换器。为此，本发明的催化剂涂层也能以被分成更小结构的形式组装，其中废气温度被最大化用于开始催化剂中的反应。因此，优选地在涡轮上游(前涡轮催化剂)或者其稍下游(预催化剂)使用例如一个或多个小催化剂胞或其它的结构(金属纤维、混合器)。催化剂涂层可以位于废气路径上的任意点、在结构(涡轮的翼部、缸体或涡轮的出口)或管道的壁上。 
如果对于下游处理而言除颗粒分离器外氧化催化剂也是必要的话，所述颗粒分离器也可以涂覆有本发明的催化剂涂层。这样，可以 获得非常紧凑的结构。颗粒分离器可以由陶瓷、金属、金属氧化物、碳化物(例如SiC)、氮化物材料或其混合物制成。所述结构可以是胞状颗粒捕捉器或棒状结构，其中沿流动方向，气体流过壁上的孔，同时颗粒被留在分离器的入口侧。其它的分离器包括纤维状、网状、泡沫状或片状结构，其也可涂覆有本发明的催化剂。除了颗粒分离外，这种结构还由于成本原因或由于它们造成的低压降而被使用。 
根据本发明的实施例，催化剂可以包括多个涂覆层叠层，其中至少一个为本发明的层。本发明的催化剂还能涂覆有本发明的另一层，或者表面层没有活性金属。该保护层能防止完全活性的金属离开催化剂，防止下面的层惰性化，促进颗粒吸收到表面，并且/或改变表面层相对于下面的层的电特性(导电性、充电等)。 
催化剂可以包括例如钪、钛、铬、锰、铁、钴、铜、镧、金、银、镓、铟和/或铈作为催化活性材料。 
基板可以优选地具有堆叠在一起的波纹片，其具有相对于彼此的倾斜角。它们也可以通过电阻焊接优选地在交叉点处连接在一起。与直通道相比，在像这样的畅通通道中物质和热量传递非常高。 
基板也可以是损伤基板，其具有压痕和/或突起。这会导致旋涡运动，从而与直通道相比产生更好的物质和热量传递。 
基板中非均匀流动能通过促进气体流过支撑物的小孔来促进颗粒在根据本发明的多孔片上减少。这种流动是由于与下面的通道间的压差产生的。另外，突起和凹陷也在基板中造成压差，从而促进气体流过根据本发明的多孔片。这种现象导致颗粒附着到支撑物上，以及更好地减少废气中的颗粒。 
基板可以是圆锥形或管状。基板的形状取决于例如发动机和废 气。 
附图说明
现在将参考附图更详细地描述本发明的一些实施例，附图中： 
图1显示具有平直多孔扳和其它的平滑波纹片的基板； 
图2显示具有波纹多孔片和其它的平直片的基板； 
图3显示具有波纹多孔片和其它的平滑波纹片的基板； 
图4显示具有连接在一起的波纹多孔片的基板； 
图5显示具有波纹多孔片、纤维片和其它的平滑片的基板； 
图6显示部分地被具有粗颗粒和纤维的支撑物覆盖的网状片； 
图7显示部分地被具有粗颗粒的支撑物覆盖的网状片； 
图8显示基本上被粗支撑物覆盖的网状片； 
图9显示基本上被粗支撑物覆盖的网状片的照片； 
图10显示网状片的横截面； 
图11显示网状片的表面剖面； 
图12显示连接在一起的网状片的三维图像； 
图13显示利用现有技术以及本发明的催化剂的测试结果；和 
图14显示带有以及不带有粗颗粒的支撑物的孔尺寸分布。 
具体实施方式
图1中基板1包括平直网状片3a和其它的平滑波纹片2a，它们连接在一起使得在它们之间有畅通通道4。图2中基板1包括波纹网状片3b和平滑平直片2b，它们连接在一起使得在它们之间有畅通通道4。图3中基板1包括波纹网状片3b和其它的平滑波纹片2a，它 们连接在一起使得在它们之间有畅通通道4。图4中基板1包括波纹网状片3b，它们连接在一起使得在它们之间有畅通通道4。图5中基板1包括波纹网状片3b、金属丝网状片5以及平滑平直片2b，它们连接在一起使得在它们之间有畅通通道4。在所有这些实施例中，气体都能流过畅通通道，并且根据压差和流体环境，气体还流过涂覆有根据本发明的粗粒材料的片，且废气中的颗粒附着到支撑物。颗粒还因为与粗颗粒以及纤维的碰撞而附着到支撑物上。优选地，所述多孔片存在两种尺寸的畅通通道。 
图6到图8显示了具有金属丝31的网状片3，其具有正方形开口32。图6中网状片3部分地被具有粗颗粒和纤维的支撑物33覆盖。图7中网状片部分地被具有粗颗粒的支撑物33覆盖。图8中网状片3的开口32基本上都被具有粗颗粒的支撑物33覆盖。这些多孔片是本发明的例子，并显示了生产和使用根据本发明的多孔片的多种可能性。 
图9是被粗支撑物43覆盖的网状片41的照片，该粗支撑物43具有大约2μm的中值颗粒尺寸。 
图10和图11中网状片3被具有细颗粒33f和粗颗粒33c的支撑物33覆盖。粗支撑物主要覆盖网状片3的金属丝31和开口32。废气G能通过支撑物33的小孔35流过网状片。废气的颗粒优选地附着到支撑物的表面上。 
图12中基板1具有连接在一起的波纹网状片3b。这些网状片可以被本发明的粗支撑物覆盖。在这些网状片之间有位于所述基板1中的畅通通道4，允许废气畅通地流过所述基板。该实施例在减少废气的颗粒中是非常优选的。 
图13显示利用现有技术催化剂和根据本发明的催化剂的测试结果。现有技术常规催化剂(DOC)具有卷在一起并用针连接的平直和波纹平滑片。支撑物具有大约1.0μm的中值颗粒尺寸，并且其中没有粗颗粒。根据本发明的催化剂(POC)具有粗支撑物，该粗支撑物具有大约2μm的中值颗粒尺寸。POC-18534具有卷在一起并具有压痕的平直网状片和平滑波纹片。POC-18535具有相对于彼此倾斜20度堆叠在一起的波纹网状片。网状片在交叉点处通过电阻焊接连接在一起。 
图14显示支撑物的测量结果。在wc500中是具有1.4μm的中值颗粒尺寸以及8nm的中值孔尺寸的常规支撑物。在wc501中支撑物包括粗颗粒，并且中值孔尺寸为3.0μm且中值孔尺寸超过10nm。 
利用根据本发明的基板颗粒的减少为33％和37％，而利用现有技术基板颗粒的减少为12％。结果高度和明确地证明了本发明的网状片以及具有该网状片的基板的效率。与利用现有技术的催化剂(4％)相比，利用根据本发明的催化剂Nox(氮氧化物)减少也很高(9％，16％)。CO减少以及THC减少对于所有催化剂而言都处在相同水平。这显示了根据本发明的催化剂除了减少颗粒外还能有效地降低废气的组分。这样的结合使得它们非常优选地适于处理内燃机的废气。 

Claims (8)

1.一种用于处理内燃机废气的金属基板，所述金属基板包括波纹网状片(3b)，所述波纹网状片(3b)连接在一起以便在它们之间有畅通通道，其特征在于，所述波纹网状片(3b)具有30到300的网目数，所述波纹网状片(3b)被支撑物(33)至少部分地覆盖，所述支撑物(33)具有孔尺寸超过10nm的中值小孔(35)以及颗粒尺寸为1.4μm到15μm的中值颗粒，并且支撑物(33)的面积质量为20到200g/m2。
2.如权利要求1所述的金属基板，其特征在于，所述波纹网状片(3b)的所有开口(32)被支撑物(33)填充。
3.如前述权利要求1或2所述的金属基板，其特征在于，支撑物(33)的中值颗粒尺寸为1.5到3.5μm。
4.如前述权利要求1或2所述的金属基板，其特征在于，所述支撑物(33)的至少一部分被碾磨过。
5.如前述权利要求1或2所述的金属基板，其特征在于，所述支撑物(33)的BET比表面积为30到300m2/g。
6.如前述权利要求1或2所述的金属基板，其特征在于，所述支撑物(33)包括纤维，纤维从所述支撑物的平面突出来。
7.一种制造用于处理内燃机的废气的金属基板的方法，所述金属基板包括波纹网状片(3b)，所述波纹网状片(3b)连接在一起以便在它们之间有畅通通道，其特征在于，所述波纹网状片(3b)具有30到300的网目数，所述波纹网状片(3b)被支撑物(33)至少部分地覆盖，所述支撑物(33)具有孔尺寸超过10nm的中值小孔(35)以及颗粒尺寸为1.4μm到15μm的中值颗粒，并且支撑物(33)的面积质量为20到200g/m2。
8.如权利要求7所述的方法，其特征在于，所述波纹网状片(3b)的所有开口(32)被支撑物(33)填充。
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