CN105074151A - 废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法 - Google Patents

废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法 Download PDF

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CN105074151A
CN105074151A CN201480017813.XA CN201480017813A CN105074151A CN 105074151 A CN105074151 A CN 105074151A CN 201480017813 A CN201480017813 A CN 201480017813A CN 105074151 A CN105074151 A CN 105074151A
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occlusion
reduction catalyst
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长冈大治
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Abstract

本发明提供一种废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法，能够判别NOx吸藏还原型催化剂的硫中毒和热劣化。该废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法为，在与发动机E的排气管(20)连接的NOx吸藏还原型催化剂(26)中，交替反复进行吸藏循环和浓还原循环，在反复进行该吸藏循环和浓还原循环的期间，在NOx吸藏率降低时进行S清除，在该方法中，预先制作表示基于经年劣化的NOx吸藏还原型催化剂(26)的吸藏循环中的NOx吸藏量的NOx吸藏映射，基于该NOx吸藏映射求出理想NOx吸藏量，另一方面根据NOx传感器值计算吸藏循环中的实际NOx吸藏量，根据该理想NOx吸藏量与实际NOx吸藏量的差来判定NOx吸藏还原型催化剂的由于硫中毒引起的劣化和热劣化。

Description

废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法
技术领域
本发明涉及使用了NOx吸藏还原型催化剂的废气后处理装置，尤其涉及废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法。
背景技术
作为柴油发动机的废气后处理装置，DOC(DieselOxidationCatalyst：氧化催化剂)、DPF(DieselParticulateFilter：柴油颗粒过滤器)、NOx吸藏还原型催化剂(LNT：LeanNOxTrap或者NSR：NOxStrageReduction)、尿素SCR(SelectiveCatalysticReduction：选择催化还原)系统等被实用化。
DOC和DPF系统是用于减少PM的有力手段。设置于废气流的前级的DOC为，虽然固体的煤烟本身无法氧化，但能够对占据PM整体的30～70％的可溶性有机成分(SOF)的大部分进行氧化，还能够同时除去HC、CO，设置于后级的DPF为，由具有细孔径的多孔质陶瓷等形成，捕捉废气中的大部分PM。
NOx吸藏还原型催化剂为，在氧化铝(Al2O3)等催化剂载体上载持有Pt、Pd等贵金属催化剂、以及Na、K、Cs等碱金属、Ca、Ba等碱土类金属、Y、La等稀土类等的具有NOx吸藏功能的吸藏材料，根据废气中的氧浓度来发挥NOx吸藏和NOx放出净化这两个功能。
基于该NOx吸藏还原型催化剂的净化系统，在通常运转状态那样废气中的氧浓度较高的条件(稀空燃比)下，废气中的NO由Pt、Pd等贵金属催化剂等氧化为NO2，吸藏材料使该NO2成为硝酸盐(Ba(NO3)2)而吸藏从而净化NOx。
但是，当持续进行NOx的吸藏时，硝酸盐饱和而失去吸藏材料的吸藏功能，因此改变运转条件，在低氧浓度的条件下，进行EGR(ExhaustGasRecirculation：废气再循环)、燃料的后喷射、排气管喷射，形成浓状态，在贵金属催化剂上使燃料还原，由此在废气中生成CO、HC、H2而使NOx还原，从而放出净化NOx。
如此，基于NOx吸藏还原型催化剂的净化系统，是在空燃比稀时(氧浓度较高的条件)吸藏NOx，在空燃比浓时对所吸藏的NOx进行还原净化的系统。
然而，作为NOx吸藏还原型催化剂劣化的主要原因，存在硫中毒和热劣化。
NOx吸藏还原型催化剂在吸附、吸藏NOx的同时还吸附、吸藏废气中的SOx，由此产生硫中毒。SOx与NOx不同，不能够容易地脱离，为了使蓄积于吸藏材料的S放出，而以使催化剂的气氛温度成为700℃以上的高温、且空燃比成为浓气氛的方式进行控制，由此Ba2SO4成为碳酸盐+SO2，而进行硫磺的脱硫。NOx吸藏还原型催化剂需要以一定的行驶间隔来进行脱硫控制(S清除)而进行再生。
热劣化是如下现象：与通常的氧化催化剂相同，载持于催化剂的贵金属由于热而凝聚而比表面积变小，由此活性降低的现象。将该现象称作烧结(sintering)。
现有技术文献
专利文献
专利文献1：日本专利第4474775号公报
专利文献2：日本特开2008-261252号公报
专利文献3：日本特开2012-87749号公报
发明内容
发明要解决的课题
但是，即使进行S清除而进行再生，也无法通过传感器来检测脱硫了的S的量，因此无法得知脱硫的量。因此，在催化剂的性能劣化的情况下，难以区分热劣化和硫中毒。
由热劣化导致的劣化是不能够恢复的，需要更换催化剂，但硫中毒存在能够恢复的可能性，因此需要提早确定劣化的原因而采取适当的措施。
对于脱硫了的S的量，通过实验来测定相对于催化剂温度和拉姆达(λ＝所供给的空气量/理论上需要的空气量)的脱硫量，将该脱硫量作为映射而保持，根据S清除时的催化剂温度和拉姆达(λ)来推定脱硫量。
但是，在实际中由于各种外部干扰而S清除时的脱硫量产生偏差，因此即使想要完全脱硫，在实际中也存在S逐渐蓄积到NOx吸藏还原型催化剂的可能性。结果，净化率会降低，而无法与热劣化区分。
因此，本发明的目的在于解决上述课题，提供一种废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法，能够判别NOx吸藏还原型催化剂的硫中毒和热劣化。
用于解决课题的手段
为了实现上述目的，本发明为一种废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法，通过与发动机的排气管连接的NOx吸藏还原型催化剂，交替地反复进行对废气中的NOx进行吸藏的吸藏循环、以及在该吸藏循环中的吸藏率降低时对所吸藏的NOx进行还原净化的浓还原循环，在反复进行该吸藏循环和浓还原循环的期间，在NOx吸藏还原型催化剂由于硫磺而中毒而NOx吸藏率降低时，进行S清除，该废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法的特征在于，预先制作表示基于经年劣化的通过NOx吸藏还原型催化剂的吸藏循环中的NOx吸藏量的NOx吸藏映射，基于该NOx吸藏映射求出理想NOx吸藏量，另一方面，根据NOx传感器值计算吸藏循环中的实际NOx吸藏量，根据该理想NOx吸藏量与实际NOx吸藏量之差，来判定NOx吸藏还原型催化剂的由硫中毒引起的劣化和热劣化。
优选为，根据随着该NOx吸藏还原型催化剂的经年劣化而NOx吸藏量相对于废气温度的关系来制作上述NOx吸藏映射，基于吸藏循环中的废气温度和累计燃料消耗量并根据上述NOx吸藏映射来求出吸藏循环中的理想NOx吸藏量。
优选为，在根据上述NOx传感器值来计算实际NOx吸藏量时，按时间对吸藏循环中的NOx吸藏还原型催化剂的入口侧的废气中的NOx浓度与出口侧的NOx浓度之差进行积分而求出实际NOx吸藏量。
优选为，如果理想NOx吸藏量与实际NOx吸藏量之差小于阈值，则判定为NOx吸藏量无异常，此外，在理想NOx吸藏量与实际NOx吸藏量之差大于阈值时，再次进行S清除，在之后的吸藏循环中，再次求出理想NOx吸藏量与实际NOx吸藏量并且将其差与阈值进行比较，在该差小于阈值时，作为通过S清除而从硫中毒恢复而判定为无异常，如果差再次大于阈值，则判定为热劣化。
发明的效果
本发明预先制作NOx吸藏还原型催化剂的基于经年劣化的NOx吸藏量的NOx吸藏映射，将根据该NOx吸藏映射求出的理想NOx吸藏量与根据NOx传感器值求出的实际NOx吸藏量进行比较，由此发挥能够判定由硫中毒引起的劣化和热劣化这种优异效果。
附图说明
图1是实施本发明的废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法的装置的概要图。
图2是表示废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法的流程图的图。
图3是在本发明中对理想NOx吸藏量和实际NOx吸藏量进行说明的图，图3(a)是表示NOx吸藏映射的图，图3(b)是表示当在NOx吸藏率降低时进行S清除时的行驶距离与NOx吸藏量之间的关系的图，图3(c)是对吸藏循环中的实际NOx吸藏量进行说明的图。
具体实施方式
以下，基于附图对本发明的优选的一个实施方式进行详细说明。
图1表示基于NOx吸藏还原型催化剂的废气后处理装置10。
在发动机E的进排气系统上连接有涡轮增压器11和EGR管12，从空气滤清器13吸入的空气由涡轮增压器11的压缩机14压缩并且朝进气通路15压送，并从发动机E的进气歧管16朝发动机E内供给。在进气通路15上设置有用于对向发动机E的空气量进行调节的进气门17。
从发动机E排出的废气，从排气歧管18排出至涡轮增压器11的涡轮19并且驱动涡轮19，并向排气管20排气。
在进气歧管16和排气歧管18上连接有EGR管12，在EGR管12上连接有用于对从排气歧管18到进气歧管16的废气进行冷却的EGR冷却器21，并且连接有调节EGR量的EGR阀22。
废气后处理装置10构成为，在涡轮19下游侧的排气管20上设置有排气管喷射器23，在该排气管喷射器23下游侧的排气管20上所形成的罐装容器24内，依次罐装有DOC25、NOx吸藏还原型催化剂26、以及DPF27。
在DOC25的上游侧设置有入口侧NOx传感器28，在NOx吸藏还原型催化剂26的入口侧设置有废气温度传感器29，在NOx吸藏还原型催化剂26的出口侧设置有出口侧NOx传感器30。
通过ECU32对发动机E进行运转的整体控制。在ECU32中形成有NOx吸藏还原型催化剂26的吸藏还原脱硫控制单元33、理想NOx吸藏量计算单元34、以及实际NOx吸藏量计算单元35。
吸藏还原脱硫控制单元33进行在空燃比稀状态下进行NOx吸藏的吸藏循环、以及在NOx吸藏率降低时通过排气管喷射器23脉冲地喷射燃料HC而在空燃比浓状态下进行NOx还原净化的浓还原循环，并且，在反复进行吸藏循环和浓还原循环的期间，在NOx吸藏还原型催化剂26由于硫磺而中毒而NOx吸藏率降低时，将废气温度提高至700℃而进行S清除。该S清除为，例如在对DPF27的PM进行了再生紧后进行，对发动机E的燃料喷射量进行控制并且对由喷射器进行的后喷射等多级喷射进行控制，并且对从排气管喷射器23喷射的燃料HC进行控制，将废气温度提高至700℃，对吸藏于NOx吸藏还原型催化剂26的SOx进行脱硫。
即，DPF27的再生为，在向DPF27堆积的PM堆积量蓄积了规定量而DPF27前后的差压达到一定时、或者在行驶了规定的行驶距离时，ECU32进行PM的自动再生控制，在进行PM再生时，进行后喷射、基于排气管喷射器23的燃料喷射而将废气温度提高至600℃，由此使向DPF27堆积的PM燃烧，使废气温度变高(约600℃)，由于在浓禁止的情况下进行该PM再生，因此在PM再生结束之后，接着通过由排气管喷射器23进行的燃料喷射将废气温度升温至约700℃而进行S清除。
理想NOx吸藏量计算单元34，基于后述的NOx吸藏映射，根据吸藏循环中的来自废气温度传感器29的废气温度以及累计燃料消耗量，求出理想NOx吸藏量。
实际NOx吸藏量计算单元35，按时间对吸藏循环中的NOx吸藏还原型催化剂26的入口侧的废气中的NOx浓度与出口侧的NOx浓度之差进行积分而求出实际NOx吸藏量。
根据图3对该理想NOx吸藏量计算单元34和实际NOx吸藏量计算单元35进行说明。
图3(a)表示NOx吸藏循环的NOx吸藏映射。
NOx吸藏量依存于催化剂温度(废气温度)，并且由于NOx吸藏还原型催化剂的经年劣化而吸藏量减少，因此预先通过实验根据NOx吸藏曲线A0求出NOx吸藏循环的初期的NOx吸藏还原型催化剂的与催化剂温度相对的NOx吸藏量，并且由于NOx吸藏还原型催化剂经年劣化，因此依次以行驶距离等为基准而求出劣化了的NOx吸藏曲线A1、A2、……An，NOx吸藏曲线An表示吸藏率降低而需要更换催化剂。该NOx吸藏映射的NOx吸藏曲线A1、A2、……An是进行了理想的脱硫时的值，求出按照经年变化的最大的NOx吸藏量。
来自该图3(a)的NOx吸藏映射的理想NOx吸藏量为，从初期的NOx吸藏曲线A0起，依次基于车辆的行驶距离、经过年数来选择NOx吸藏曲线A1、A2、……An，基于该选择的NOx吸藏曲线并根据NOx吸藏循环时的温度和吸藏循环中的累计燃料消耗量，来求出理想NOx吸藏量。
图3(b)表示在反复进行NOx的吸藏循环和浓还原循环的期间，在NOx吸藏还原型催化剂由于硫磺而中毒而NOx吸藏率降低时，进行S清除时的行驶距离与NOx吸藏量之间的关系。
在图3(b)中，L表示相对于经年变化(行驶距离)的NOx的吸藏循环时的理想NOx吸藏量曲线，当相对于该理想NOx吸藏量曲线的理想NOx吸藏量而吸藏量减少值d的量时，按照行驶距离来说行驶了1000km程度时，NOx吸藏还原型催化剂由于硫磺而中毒，吸藏性能降低了值d的量，为了使其NOx吸藏性能恢复而进行S清除(S/P)。在进行该S清除的时期，废气中的SOx浓度最大为7ppm程度，NOx吸藏还原型催化剂吸藏该SOx的量使NOx吸藏量降低值d的量，因此能够根据车辆的发动机运转状况和行驶距离、或者到此为止的累计燃料消耗量来求出理想NOx吸藏量。
此外，图3(b)的理想NOx吸藏量曲线的虚线中的值An表示：即使进行S清除，NOx吸藏还原型催化剂也热劣化，即便使吸藏性能恢复值d的量，NOx吸藏性能也不恢复的催化剂更换时期。
图3(c)是对基于实际NOx吸藏量计算单元35的吸藏循环中的实际NOx吸藏量进行说明的图。
通常，通过入口侧NOx传感器28对朝NOx吸藏还原型催化剂流入的废气中的NOx浓度进行检测，NOx浓度大致为200ppm程度，为了方便而在图中表示为在200ppm恒定。此外，通过出口侧NOx传感器30对出口浓度进行检测，因此该出入口浓度差成为由NOx吸藏还原型催化剂吸藏的量。因此，能够通过按照在进行了浓还原净化之后、到进行下一次浓还原净化之前的吸藏循环中的时间对该出入口NOx浓度差进行积分，来计算实际NOx吸藏量，即能够将图3(c)的用网格表示的区域作为实际NOx吸藏量进行计算。
在本发明中，能够根据图3(a)、图3(b)求出切换至浓还原净化之前的吸藏循环中的理想NOx吸藏量，并且根据图3(c)求出该吸藏循环中的实际NOx吸藏量，对这两者之差进行计算，并根据该差来判定NOx吸藏还原型催化剂的由硫中毒引起的劣化和热劣化。
即，由硫中毒引起的NOx吸藏量的降低，如图3(b)所示，在相对于该吸藏循环的理想NOx吸藏量降低了值d的量时进行S清除，将该值d作为阈值，如果理想NOx吸藏量与实际NOx吸藏量之差小于阈值则判定为无异常，此外，在差为阈值以上时，为了判定是由于热劣化而NOx吸藏量降低、或者是由于上次的S清除中的脱硫不充分而NOx吸藏量降低，而再次强制性地进行S清除，在该S清除结束之后，进行吸藏循环，在该吸藏循环中求出理想NOx吸藏量和实际NOx吸藏量，将其差与阈值进行比较，如果低于阈值，则上次的判断作为由于硫中毒引起的劣化而判定为无异常。此外，在即使进行S清除、差仍为阈值以上而吸藏性能不恢复时，判断为不能够恢复的催化剂劣化，而进行OBD(On-boardDiagnotics：车载诊断)显示。
接着，根据图2对本发明的流程进行说明。
在步骤S10中开始控制，在步骤S11中，保持进行了理想的脱硫的情况下的NOx吸藏映射，按照每个吸藏循环计算根据该NOx吸藏映射和累计燃料消耗量求出的理想NOx吸藏量、与根据由NOx传感器值求出的NOx传感器值而进行校正后的实际NOx吸藏量之差。
接着，在步骤S12中，根据S清除实施开始判定，基于在步骤S11中计算出的差，在差小于S清除开始时，作为不符合条件而返回到步骤S11，再次反复进行吸藏循环和浓还原净化循环而计算差。
在步骤S12中，在理想NOx吸藏量与实际NOx吸藏量之差成为一定以上时，开始S清除，根据S清除的结束判定使S清除结束。
之后，如果S清除结束，则在步骤S13中，再次对理想NOx吸藏量与由NOx传感器求出的实际NOx吸藏量之差进行计算。
如果该值小于阈值则判断为吸藏量无异常，作为符合条件而结束控制(步骤S16)。
在步骤S13中，在理想NOx吸藏量与实际NOx吸藏量之差为阈值以上时，在步骤S14中，再次进行S清除，并对理想NOx吸藏量与由NOx传感器求出的实际NOx吸藏量之差进行计算。
在步骤S14中，如果该差值小于阈值(符合条件)，则判断为从由于硫中毒引起的劣化恢复，并结束控制(步骤S16)。
此外，在步骤S14中，如果该差值为阈值以上(不符合条件)，则在步骤S15中，判断为即使进行S清除性能也不恢复、即不能够恢复的催化剂劣化，在进行了OBD的催化剂故障的显示之后，结束控制(步骤S16)。
如此，根据本发明，无需追加的传感器等，就能够区分NOx吸藏还原型催化剂的热劣化和硫中毒。
由于能够判断是否能够恢复而能够采取适当的措施(S清除或者OBD显示)，因此能够防止废气的恶化、由浪费的浓空燃比引起的燃料消耗率恶化。
符号的说明：
20：排气管；26：NOx吸藏还原型催化剂；E：发动机。

Claims (5)

1.一种废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法，
通过与发动机的排气管连接的NOx吸藏还原型催化剂，交替地反复进行对废气中的NOx进行吸藏的吸藏循环、以及在该吸藏循环中的吸藏率降低时对所吸藏的NOx进行还原净化的浓还原循环，在反复进行该吸藏循环和浓还原循环的期间，在NOx吸藏还原型催化剂由于硫磺而中毒而NOx吸藏率降低时，进行S清除，
该废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法的特征在于，
预先制作表示基于经年劣化的通过NOx吸藏还原型催化剂的吸藏循环中的NOx吸藏量的NOx吸藏映射，基于该NOx吸藏映射求出理想NOx吸藏量，另一方面，根据NOx传感器值计算吸藏循环中的实际NOx吸藏量，根据该理想NOx吸藏量与实际NOx吸藏量之差，来判定NOx吸藏还原型催化剂的由硫中毒引起的劣化和热劣化。
2.如权利要求1所述的废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法，其中，
根据随着该NOx吸藏还原型催化剂的经年劣化而NOx吸藏量相对于废气温度的关系来制作上述NOx吸藏映射，基于吸藏循环中的废气温度和累计燃料消耗量并根据上述NOx吸藏映射来求出吸藏循环中的理想NOx吸藏量。
3.如权利要求1所述的废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法，其中，
在根据上述NOx传感器值来计算实际NOx吸藏量时，按时间对吸藏循环中的NOx吸藏还原型催化剂的入口侧的废气中的NOx浓度与出口侧的NOx浓度之差进行积分而求出实际NOx吸藏量。
4.如权利要求1至3中任一项所述的废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法，其中，
如果理想NOx吸藏量与实际NOx吸藏量之差小于阈值，则判定为NOx吸藏量无异常。
5.如权利要求4所述的废气后处理装置中的NOx吸藏还原型催化剂的劣化判定方法，其中，
在理想NOx吸藏量与实际NOx吸藏量之差大于阈值时，再次进行S清除，在之后的吸藏循环中，再次求出理想NOx吸藏量与实际NOx吸藏量并且将其差与阈值进行比较，在该差小于阈值时，作为通过S清除而从硫中毒恢复而判定为无异常，如果该差再次大于阈值，则判定为热劣化。
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