CN106460628A - 检测催化转化器老化程度的方法 - Google Patents
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Abstract
本发明涉及一种测定催化转化器(2)老化状态的方法。所公开的方法以非接触方式运行,当使用高频电磁波激发位于壳体中的所述催化转化器(2)时,分析所形成的谐振。
Description
具体实施方式
本发明提出了一种测定催化转化器老化程度的方法。目标方法通过分析在利用高频电磁波激发布置于壳体内的催化剂时形成的谐振来无接触地起作用。
日益严格的废气法律,伴随着减少燃料消耗的压力,促使人们必须针对内燃机以及内燃机废气处理找到新方法。这也意味着用于控制和监测排放控制系统的新方法。
例如,在汽油发动机(所谓的λ=1发动机)中,使用第一λ传感器检测未处理废气的空气/燃料比λ(也称为空气比)。在相对于标称值λ=1存在控制偏差的情况下调节空气/燃料比。λ=1必须或多或少地随时间推移保持均值。考虑到布置在第一λ传感器之后的所谓“三效催化转化器”的储氧能力,只要该催化转化器仍处于良好状态,就总是发生最佳转化。当催化转化器的品质下降(这尤其会通过有害废气HC、CO和NO的转化率下降和启动温度升高表现出来)时,该催化转化器的储氧能力也下降。布置在该催化转化器之后的第二λ传感器可检测此问题。这种间接方法需要非常复杂的建模,其中储氧催化转化器的状态是从两个λ传感器的信号推断的,其建模尤其需要发动机操作状态模型(参见例如J.Riegel etal.,“Exhaust gas sensors for automotive emission control”Solid State Ionics152–153(2002),783–800(J.Riegel等人,“用于汽车尾气排放控制的废气传感器”,《固态离子学》,152-153,2002年,第783-800页))。
其他类型的催化转化器,例如柴油机(氧化催化转化器)、包覆颗粒过滤器、NOx储存催化转化器和SCR催化转化器,均会出现老化现象,这导致催化转化器的转化效率随操作时间推移而持续降低。因此,有必要使用OBD测量设备进行适当监测,以便能够辨识和更换(如果必要的话)不能再充分处理废气的催化转化器。
在这方面的辅助具体是通过一些方法来提供的,在所述方法中可直接测定催化转化器的操作状态和品质,特别是在常规操作期间。可由此测定催化转化器的功能仍然可用的程度,如例如R.Moos,M.Wedemann,M.S.Reiβ,G.Fischerauer,“Direct CatalystMonitoring by Electrical Means:An Overview on Promising Novel Principles”,Topics in Catalysis,52(2009),2035-2040(R.Moos,M.Wedemann,M.S.Reiβ,G.Fischerauer,“用电气手段进行直接的催化剂监测:关于有前途的新颖原理的综述”,《催化论题》,第52卷,2009年,第2035-2040页)能够展示的。高频辅助系统,如例如DE102011107784A1、DE102008012050A1或DE10358495A1中所公开的,具有特别简单的设计。
在申请DE10358495A1中,提出了一种用于识别催化转化器(特别是NOx储存催化转化器)的状态的无接触方法。为此,在设计为空腔谐振器的催化转化器壳体的内部激发电磁微波谐振,并且观测谐振频率和/或品质的偏移。将谐振频率的降低被作为储存材料中NOx负荷增加的量度。一旦达到谐振频率的预定值,就进行再生。
在DE102008012050A1中,在设计为空腔谐振器的催化转化器壳体的内部激发电磁微波谐振,并且例如观测谐振频率的位置。将例如谐振频率的变化作为催化转化器的储存材料中的氧负荷的量度。
期望得到一种普遍适用、同样简单且稳健的方法,通过该方法可充分和可靠地测定所有(如果可能的话)汽车废气转化器的品质或转化效率。
通过具有本发明权利要求1的特征的方法实现了这些目标以及对于本领域的技术人员从现有技术显而易见的其他目标。在从属于权利要求1的从属权利要求中,提供了根据本发明的方法的其他优选实施方案。
以非常有利的同时还成功实现所提出目标的方式,利用在催化转化器温度小于200℃时的谐振特性来测定催化剂表面上的水吸附,并且由此以如下方法推断催化转化器的老化:通过优选地在微波范围内发射交变电磁场并检测该交变电磁场,来非侵入性地检测位于金属的催化转换器壳体中的汽车废气转化器的老化。
汽车废气转化器的表面因热应力或污染而变化。在此过程中,可发生反应的自由表面位置的数量减少。在受到污染的情况下,活性中心被阻断,而如果是受热应力的作用,则微细分布的贵金属和载体材料均会被烧结在一起。表面由此因老化而缩小,并且相应地其在表面上化学和物理吸附物质的能力也降低。因老化而减少的自由表面位置的量改变了表面上可吸附的水量。此外,表面上可吸附的水量一方面取决于废气中水的比例,另一方面取决于温度。催化转化器(包括载体材料)的电磁材料参数(导电率和介电常数或复介电常数)因水吸附而改变。
因此,在给定的催化转化器温度下测定相应的谐振特性,或者在给定的温度范围(例如df谐振/dT)内追踪相应的谐振特性,然后与更新(younger)或更新制(fresher)状态的催化转化器的数据进行比较,该更新或更新制状态的催化转化器的数据可保存在汽车的ECU中。如果结果向更低的值偏移,例如在谐振频率随温度变化的情况下,则催化转化器因其可吸收更少的水而被假定为老化,并且空腔谐振频率相应地改变。然而,充分的区分仅发生在低于200℃的温度下。因此,测量优选地在大于50℃和小于200℃、优选地在60℃和150℃之间、特别优选地在70℃和120℃之间进行。此温度范围也是有利的,因为由于电性质在该温度范围内几乎不随氧负荷变化(如DE102011107784A1中的图4所示),所以DE10358495A1中描述的状态诊断至少对于三效催化转化器不适用。在根据本发明的方法中,如果可能的话,应该排除或校正环境影响,例如利用排气系的加热特性。例如,可通过DE102011107784A1中概述的方法来校正温度影响。
如已指出的,被照射腔的谐振特性在车辆运行期间随着位于车辆中的催化转化器的吸附能力而改变。这相应地又取决于催化转化器的老化程度。优选地,将被吸附的试剂是水;当然,在发生燃料燃烧时,水总是自然而然地存在于废气中。水还具有高介电常数,并使得催化转化器的电磁材料参数随着吸附增多或减少而改变至相应程度。除了老化之外,所吸附水的量还受废气中水含量的影响。有利的是,由此在发动机控制中计算废气中的水含量,并且在根据谐振信号确定老化程度时将废气中的水含量考虑在内。如果废气中的水含量随时间推移变化,则可通过考虑水的有限吸附速率来进一步改进评估。优选地,当废气中存在足够和最好是恒定量的水时采用根据本发明的方法。特别优选地,当存在每体积含有3-20份水、优选地每体积含有5-15份水的废气混合物时进行测量。
催化转化器的电特性不仅可利用谐振频率测定,还可通过考虑其他谐振特性来测定。此类特性优选地选自以下各项:谐振频率、振幅、谐振器品质(Q)、损耗、散射矩阵Sij的参数、透射因数的量值、谐振峰或谐振谷的宽度以及从S参数获得的其他量(参见DE102008012050A1)。在该语境中,谐振频率以及反射参数S11或透射参数S12量值是特别优选的。在该语境中,使用谐振频率进行评估(参见图2)是特别优选的。还可使用各种谐振模式。特别地,对不同的干扰变量(如温度)有不同反应的那些是优选的。
汽车催化转化器的特征在于:由于精细分布的贵金属如Pt、Pd或Rh,它们提供较大表面,在该表面上化学反应发生的更快。同样,如上所述,本发明方法基于以下事实:谐振特性随着催化转化器的不断老化而变化。本文所考虑的催化转化器都是与本领域的技术人员相关的那些,因为所有催化转化器都遵循相同的原理。选自以下项的那些催化转化器是优选的:三元催化转化器、柴油氧化催化转化器(可能是催化包覆的柴油颗粒过滤器)、NOx储存催化转化器和SCR催化转化器。在本文的上下文中,具有储氧材料的三元催化转化器是特别优选的。
在本发明的一个优选实施例中,催化转化器被微波反射器(3、4)包围(DE102008012050A1)。满足以下条件的所有材料都适用于此:以最佳的低的反压力抵消废气流,并仍然能够反射所采用的微波。本领域的技术人员了解相关设备。在不确定的情况下,可使用简单的金属栅格。由此产生了在高频方面明确限定并且与连接管形状无关的谐振器。这可能是有利的,因为在催化转化器壳体和连接管之间(具体地讲在气体入口处)的圆锥形过渡部是在考虑流动和无反射的情况下设计的,例如以使得气体均匀地流经陶瓷蜂窝体。然而,从原理上讲,其中正常安装有催化转化器的相应的金属的催化转换器壳体即适用于此目的。因此,在没有反射栅格的情况下进行操作是可能的,但在某些情况下,可能需要更大的努力,这是因为催化转化器状态和所测量S参数之间的关系发生了反转。
优选地,在催化转化器(2)前后布置有一个或多个天线(5、6)(图1)以用于发送和接收电磁辐射,所述电磁辐射有利地在微波范围内。然而,根据本发明的方法也是优选的,其中使用位于金属的催化转换器壳体中的天线。该天线发送和接收相应的信号。可根据本领域的技术人员的判断来选择天线。此类设备和信号检测单元以及相应的分析单元是本领域的技术人员充分已知的(诸如出自P.S.Neelakanta,Handbook of ElectromagneticMaterials.CRC Press,Boca Raton etc.,1995(P.S.eelakanta,《电磁材料手册》,CRC出版社,波卡拉顿等,1995年)和S.H.Chao,Measurements of microwave conductivity anddielectric constant by the cavity perturbation method and their errors,IEEETransactions on Microwave Theory and Techniques 33(1985)519-526(S.H.Chao,“通过腔扰动法测量微波传导率和介电常数及其误差”,《IEEE微波理论与技术汇刊》,第33卷,1985年,第519-526页),以及其中所引用的文献)。
本发明成功地以特别有利的方式确定任何类型的废气催化转化器的老化程度。在优先权日之前,尚不知晓可通过研究催化转化器在特定温度范围内的水吸附能力来得出关于催化转化器品质的结论。本发明使用相关方法首次向本领域的技术人员提供了一种方法,借助于该方法,本领域的技术人员可以相对简单的方式在正常驾驶条件下非侵入地直接测定汽车废气转化器的老化程度。鉴于已知的现有技术领域,这绝不是显而易见的。
实例:
图1示出了废气处理系统的基本结构,该基本结构具有:壳体部分(1),其中安装有催化转化器(2);具有两个天线(5、6)(其中一个是任选的)的测量系统;控制器(7)和评估电子装置(8);以及任选的温度传感器(参见DE102008012050A1);以及任选的反射器(3、4)。
图2示出了在合成气体装置中所测量的1”×3”直径的TWC钻芯的谐振频率曲线。测量了钻芯。首先在新制时进行测试,然后在850℃下进行12小时燃料切割老化(老化1)后测量,并在1050℃下老化(老化2)后测量。在所有三种老化阶段中,催化转化器首先在还原条件下以温度斜率(20K/min)升温至600℃(λ=0.95)进行预处理,然后在氮气气氛中冷却至80℃。在实际测试期间,设定含有10%H2O的恒定合成稀燃废气(λ=1.02)。开始时,将温度在80℃下保持600s,然后以20K/min升温至600℃。将三次测试中测得的谐振频率和催化转化器的温度绘制于图2中。将N2切换成含水气氛后,可看到显著的谐振频率变化,其取决于老化程度和由此改变的催化转化器的吸附性质。谐振频率变化还取决于最高至约200℃的温度。
根据图2中的测量数据,例如评估了80℃和100℃之间的谐振频率变化,并评估了80℃下的谐振频率(表1)。
表1:
Claims (5)
1.一种方法,用于通过发射交变电磁场并检测所述交变电磁场来非侵入地检测位于金属的催化转换器壳体中的汽车废气转化器的老化程度,其中使用在小于200℃的催化剂温度下的某些谐振特性测定所述催化剂表面上的水吸附,并且由此推断所述催化转化器的所述老化程度。
2.根据权利要求1所述的方法,
其特征在于:
使用大于50℃的温度。
3.根据权利要求1和/或2所述的方法,
其特征在于:
在测量期间提供含有3体积%至20体积%的水的废气混合物。
4.根据权利要求1-3所述的方法,
其特征在于:
所用的那些谐振特性选自以下项:谐振频率、振幅、谐振器品质(Q)、损耗、散射矩阵Sij的参数以及基于这些的量(以及在不同频率范围内的量)。
5.根据权利要求1-4所述的方法,
其特征在于:
使用了天线,其位于金属的催化转换器壳体中。
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