CN102575546A - 排放控制的改进 - Google Patents
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Abstract
当启动火花点火内燃机时,用于捕集随后释放未燃烧的烃的烃捕集器如果暴露于正常温度排气则对降解敏感。本发明通过以下提供了HC捕集器的机上诊断:在HC捕集器材料中结合热敏氧储存材料,以及使用OSC效率的常规测定来确定是否HC捕集器材料已暴露于过度的温度。
Description
相关申请
本申请要求2009年9月3日提交的英国专利申请号0915326.3的优先权,该专利申请整体通过引用结合到本文中。
发明领域
本发明涉及排放控制的改进,更具体地,本发明涉及控制来自内燃机的管制排放的改进。
发明背景
本发明具体应用于火花点火内燃机,并且将关于汽油-燃料的内燃机进行描述,但是可适用于类似的发动机,例如以醇、醇-汽油共混物和液化石油气(LPG)作为燃料的那些。目前对于汽油发动机的管制排放涉及未燃烧的烃(HC)、一氧化碳(CO)和氮氧化物(NOx)。虽然通过传统三路催化剂(TWC)的废气后处理,结合空气-燃料比率的发动机管理,实现所有这些污染物的有用降低,但是全世界日益严格的规章已提出一些问题。例如,在启动时和在TWC“点火”前(即,在TWC达到其操作温度之前),HC排放有效地未经处理。“点火”可描述为催化剂以期望的转化活性催化反应的温度。例如“CO T50”为对于给定的催化剂,催化剂以至少50%效率将进料气体(例如,废气)中的一氧化碳催化转化为二氧化碳的温度。类似地,“HC T80”为烃(可能是具体的烃,例如辛烷或丙烯)以80%或更大的效率转化为水蒸汽和二氧化碳的温度。
在预点火时期来自废气管中的HC排放优选防止离开废气***。实现该目的一项提议是在该时期期间在吸收剂材料中吸收HC排放或“HC捕集”。例如,JP 8-10566公开了一种催化剂-吸附剂,其中将有效用于降低在内燃机废气中的CO、HC和NO的催化剂材料与在冷排放启动期间捕集烃的吸附剂材料组合。捕集的HC随后从捕集材料中释放,用于在TWC已达到其HC点火温度之后,通过TWC处理(即,转化为CO2和水)。另外,在JP 62-5820中,吸收剂与催化剂组合使用,使得在低温下与废气一起排放的烃被吸收剂吸收,而在高废气温度下,由发动机排放的烃与由吸收剂释放的烃一起被催化剂纯化。
催化转化器上游的汽油发动机废气的典型的温度通常超过800℃,并且可明显更高。此外,通过经过与排气歧管密切偶联的催化剂(例如小的启动催化剂)也可升高排气温度。因此,在这类装置中提出用作HC吸收剂的材料需要高温稳定性,其实例包括γ氧化铝、多孔玻璃、活性炭等。
然而,这些材料对于HC不具有足够的吸收性,并且在高温下失去很多吸收性。当废气温度在吸收性开始降低的温度和通过催化剂纯化开始可用的温度之间的范围内时,烃排放,既未被吸收剂吸收,也未被催化剂纯化。因此,在催化转化器的上游侧提供的常规HC捕集器不是非常有效,原因在于在吸收剂下游侧上提供的催化转化器变得具有活性之前,被吸收剂吸收的烃再次释放,由此使得这种烃未经纯化即排放到大气中。
与上述高温材料相比,已知沸石具有优良的HC吸收性。此外,已知不同的方法来改进HC吸附的性能和沸石稳定性。例如,JP 08-099033公开了一种HC捕集器,其包含银、IIIB族元素(例如铈、镧、钕或钇)和沸石。银改进HC吸附,特别是相对高温HC吸附,而IIIB族元素改进沸石的水热稳定性。
然而,大多数有用的沸石在火花-点火发动机的典型的废气温度下不稳定。为了补偿降低的温度稳定性,包含沸石材料的HC捕集器常规地位于TWC的下游,使得在接触HC捕集器之前将废气温度冷却。然而,这种装置需要另外的废气***组件,例如放置在HC捕集器更下游的氧化催化剂,以转化释放的烃。(参见,例如,US 6074973,公开了一种催化的HC捕集器,其包含在沸石(例如ZSM-5)上分散的银,其中HC捕集器布置在TWC的下游)。
在Keisuke Sano等人的SAE文章2007-01-0929“HC Adsorber System for SULEVs of Large Volume Displacement (用于大体积位移的SULEV的HC吸附器***)”以及在EP 0424 966A中也已提出,使用一种或另一种形式的旁路***,使得仅当需要时使用捕集器,并且不暴露于超过沸石捕集材料开始降解的温度下的大体积废气。旁路装置中的HC捕集器可仅达到例如100-300℃。现在认为结合旁路的这种HC捕集器是必要的,以满足即将到来的排放规章。
此外,“机上(on-board)诊断”***(OBD)现在是强制的,用来向车辆司机显示何时TWC失效或以降低的效率操作。进行TWC的OBD的一种有效的方法是测量TWC的氧储存组件(OSC)的效率,以及如果效率降至低于预定值则触发失效信号。在TWC中结合的现有技术水平的OSC需要在至少850℃的汽油废气温度下具有长期稳定性。出于该原因,OSC通常为高度稳定的二氧化铈-氧化锆混合氧化物,通常具有另外的稳定,所述稳定通过用另外的稀土氧化物(例如钕和/或镧的氧化物)掺杂二氧化铈-氧化锆提供。
发明概述
然而,现有的OBD技术不容易与HC捕集器一起使用,因为基于沸石的HC-捕集器通常不结合对低于保持捕集器的稳定性所需的最大温度的温度敏感的OSC。也就是,即使HC-捕集器含有常规的TWC组件,但是在暴露于比沸石降解温度显著更高的温度之后,TWC组件在OSC测试中只能失败。因此,本发明的一个目的是提供一种具有用于提供OBD的装置的HC捕集***。优选的实施方案可在相对低的温度(例如,100-300℃范围)下提供OBD检测,用于在旁路装置中布置的HC捕集器。
因此,本发明提供了一种用于处理来自火花点火内燃机的废气的HC捕集***,其中所述***结合HC吸收剂材料和牺牲性OSC材料,该HC吸收剂材料具有优良的HC吸收,该牺牲性OSC材料选为在环境温度和操作温度之间失去氧储存容量,在该操作温度下对温度敏感的吸收剂材料已降解,并且不捕集HC,例如不足够捕集HC以满足相关的排放标准。对于并线(in-line)(即,非旁路)装置,操作温度可适当低于约800℃,但是对于用于旁路应用,也可适当大于约100℃,例如大于约150℃,大于约200℃或大于约250℃。
附图简述
为了更充分地理解本发明,参考附图来描述说明性实施方案,其中:
图1为显示HC捕集器的氧储存容量的数据图;
图2为显示HC捕集效率和氧储存的数据图;和
图3为显示根据本发明的一个优选实施方案的排气处理***的组件的图。
发明详述
在一个优选的实施方案中,HC捕集器和TWC布置在单独的外壳中。如图3所示,这些外壳通过导管流体连通。在这里,发动机20产生含有HC、NOx等的废气。流通导管30用于,当废气的温度超过TWC 60的HC点火温度时,引导来自发动机的废气通过TWC 60随后通过其它导管70,例如排气管。在废气达到HC点火温度之前,例如在启动后片刻,将废气引向旁路***40,该旁路***40包含入口41、出口42、旁路导管43和HC捕集器50。在某些实施方案中,旁路***还包含布置在所述入口41和所述HC捕集器50之间的第二TWC。在这样的***中,第二TWC与HC捕集器相邻或密切接近。活页阀44布置在流通导管30、旁路导管42中、入口41处、或在可用于将至少一部分来自流通导管30的废气的流动有效转向旁路导管42的任何其它位置处。废气流动的方向用箭头表示。本文使用的术语“上游”和“下游”是指在***的正常操作中废气流动的相对方向。
可通过活页阀操纵废气通过***的流动,该活页阀可通过电子控制模块来控制。活页阀可为在废气接触TWC之前,可有效引导一部分或全部废气通过HC-捕集器的任何合适的阀或装置。
在操作中,HC捕集器可在发动机启动时操作,以吸收烃,直至发动机废气达到阈值温度,例如低于HC捕集材料的最大操作温度的温度。当废气温度超过阈值温度时(该阈值温度可为例如约300℃或约250℃),期望引导废气流动,以旁过HC捕集器,以避免被吸收剂吸收的烃由此释放。当废气的温度进一步升高至TWC的点火温度(例如约350℃)时,随后再一次废气可或应期望通过吸收剂,以释放被吸收剂吸收的烃,由此使吸收剂再生。这样释放的烃现在将被吸收剂捕集器的下游侧提供的催化转化器所含的催化剂纯化。由于当废气从吸收剂释放时,废气的温度由于吸热相转化而稍微下降,因此期望当吸收剂捕集器入口的废气的温度高于点火温度时,进行流动路径的转换,使废气再次流动通过吸收剂捕集器,以确保在催化转化器入口的废气也超过点火温度。在被吸收剂吸收的烃已释放之后,即,已使吸收剂捕集器再生,期望流动路径再次变换,以便让废气旁过吸收剂捕集器,以避免超过HC捕集器的操作温度。
本发明还提供了一种如上所述的HC捕集***,结合用于确定HC捕集***的氧储存容量的传感器45,以及电子控制模块,使得当电子控制模块接受来自传感器装置的指示氧储存容量的信号时,能确定是否牺牲性OSC组件已暴露于HC捕集材料已降解的温度。
本发明另外提供了一种用于HC捕集器的OBD的方法,所述方法包括在HC捕集材料内结合牺牲性OSC,该牺牲性OSC在最高约800℃的温度下的氧储存容量降低,并优选在小于约300℃下,通过测量HC捕集材料的氧储存容量来确定是否HC捕集器已暴露于HC捕集材料已降解并且不再对HC捕集有效的温度,即,满足相关的排放标准。用于OBD方法的理想的OSC的氧储存容量将和HC捕集器(例如沸石)组件同时或大约同时急降(collapse),使得OSC活性的降低指示可标记的HC捕集功能度的显著降低,从而HC捕集器作为整体可进行更换。这可由下文实施例8的优选的HC捕集器看到,其中相对于新鲜材料,在约800-约900℃老化之后,优选的Ag/CeO2 OSC显示氧储存容量显著降低,并且该OSC活性降低与HC捕集效率降低相关。
用于OBD***和方法的牺牲性OSC的另一个重要的方面是灵敏度。在旁路位置的HC捕集器通常在低于约350℃下切断废气流动,因此用于旁路应用的优选的牺牲性OSC也在小于约350℃下具有OSC灵敏度。相对于单独的Ag或单独的CeO2,优选的Ag/CeO2牺牲性OSC在小于约350℃下提供能证实的氧储存容量(注意在200-350℃下测量的OSC的趋势)(参见实施例7)。在小于约350℃下提高的能证实的OSC灵敏度允许更精确的OBD确定,并且在具有较低灵敏性OSC的***上避免昂贵的“假阳性”。
关于HC捕集材料本身对降解的温度灵敏度,技术人员可通过常规实验来选择用于本发明的合适的牺牲性OSC。然而,目前提出,牺牲性OSC发现于二氧化铈或二氧化铈-氧化锆混合氧化物(特别是未经例如稀土稳定的那些)中以及在某些锰混合氧化物(例如锰-氧化锆和锰-二氧化钛,或优选锰-铝酸盐)中。这种锰混合氧化物OSC描述于例如US 2004/0132615A1。这种牺牲性OSC不旨在为穷举的列举。
目前优选的HC捕集器,特别是用于旁路应用,包含银、铈源和分子筛。我们非常意外地发现,银降低可测量铈源的OSC活性的温度,因此HC捕集器的OBD可在较低的温度暴露下监测。此外,银在约800-约900℃下严重烧结,因此将存在相应的OSC水平的降低,在相同的温度范围内,捕集性能大大降低,因此OBD***可更容易地确定烃捕集的条件。银提供以下双重作用:(i) 促进在HC捕集材料上的HC吸附;和(ii) 促进OSC材料,以提供与任选布置在旁路位置的HC捕集器相关的温度范围的改进的响应。
用于优选的实施方案的合适的铈源包括原样二氧化铈(CeO2)、未经稳定的二氧化铈-氧化锆和在HC捕集制剂内的组分(例如沸石)上负载的可溶性Ce盐。
分子筛可为铝硅酸盐沸石或同种型例如SAPO。本发明预期一种或多种不同的分子筛的混合物,包括两种或更多种不同的SAPO和两种或更多种不同的铝硅酸盐沸石的共混物、两种或更多种不同的铝硅酸盐沸石的共混物或两种或更多种不同的SAPO的共混物。
用于本发明的合适的分子筛具有国际沸石协会框架类型编码(Framework Type Code)MFI、BEA、FAU、MOR、FER、ERI、LTL和CHA。目前优选的装置将铝硅酸盐沸石ZSM-5 (MFI)和β(BEA)组合。还可使用沸石Y(FAU)。
可适当选择分子筛的二氧化硅:氧化铝比率(SAR),以反映在关注的温度范围内HC捕集器的老化,这还反映在OSC降低,以提供更大的OBD灵敏度。对于ZSM-5,合适的SAR例如为·约80,而对于沸石Beta,优选的SAR为·约150。
用于本发明的优选的HC捕集器的银含量可为约0.1-约30重量%,优选约0.1-约15重量%,约1-约10重量%,和约5-约10重量%,基于烃捕集涂层的总重量。在实施方案中,催化剂中的银负载可为约5-约1750 g/ft3,优选约50-约750 g/ft3或约250-约500 g/ft3。
在某些实施方案中,铈源的含量可为涂层重量的1-75%,优选涂层重量的约5-约40 %,更优选约10-约35%或约15-约25%。在其它实施方案中,铈源可为0.1-10%。
氧储存容量可按mg/升量化。在实施方案中,例如,优选的含银的HC捕集器实施方案,新鲜状态下OSC在约100-约500 mg/l范围内。
相信本发明可具体用于混合动力驱动-火车(包括电动机),即,包括在整个驱动周期期间不必与轮子机械连接的火花-点火内燃机的那些。对于包括在整个驱动周期期间与轮子机械连接的火花-点火内燃机的常规车辆,HC捕集器可在冷启动后吸附烃,并解吸捕集的烃,用于在下游三路(three-way)催化剂或其它氧化催化剂上燃烧。HC捕集器可布置于旁路装置中,使得在冷启动烃已解吸之后,HC捕集器不暴露于较高的温度。当车辆从电池推进模式切回或从发动机用于产生电力以“装满”耗尽的电池时切回时,混合动力装置可引起火花点火发动机从冷或从“冷却”经驱动周期重复运行。
实施例
实施例1 - HC捕集器的制备
通过将β沸石浆料和ZSM-5沸石浆料与胶态二氧化硅混合得到1:1:1重量比率的β:ZSM-5:二氧化硅,来制备烃捕集器涂层(washcoat)。将另外的水和流变学改性剂随后加入到涂层中,以产生涂层A。使用在US7147892 (Aderhold等人,2006)中描述的方法,将涂层A涂布在尺寸为4.16×4.5",胞孔(cell)密度为400/6的陶瓷蜂窝基材上。涂层随后于100℃下干燥,随后于500℃下在空气中煅烧,以产生HC捕集器A。已煅烧的HC捕集器A的涂层负载为3 g/in3。
实施例2 - HC捕集器的制备
通过将高表面积未掺杂的二氧化铈加入到涂层A中,产生涂层B。如实施例1所述将涂层B涂布在陶瓷基材上,以产生HC捕集器B。已煅烧的HC捕集器B的二氧化铈负载为0.6 g/in3。
实施例3 - HC捕集器的制备
通过将硝酸银加入到涂层A,产生涂层C。如实施例1所述将涂层C涂布在陶瓷基材上,以产生HC捕集器C。已煅烧的HC捕集器C的银负载为250 g/ft3。
实施例4 - HC捕集器的制备
通过将硝酸银加入到涂层B,产生涂层D。如实施例1所述将涂层D涂布在陶瓷基材上,以产生HC捕集器D。已煅烧的HC捕集器D的银负载为250 g/ft3。
实施例5 - HC捕集器的老化
为了确定在暴露于高温废气之后烃捕集器的性能,将烃捕集器在水热气氛中老化。该气氛由10% H2O、2% O2和余量的氮气组成。于800或900℃下进行老化5小时。
实施例6 - HC捕集器储存效率(烃)
测量在车辆的冷启动期间的烃储存效率。将HC捕集器A至D安装到车辆的排气***中,将发动机冷启动,即,发动机油和发动机冷却剂在21.5-24.5℃温度范围内。通过测量在发动机空转运行20秒的同时,在HC捕集器的入口和出口处的废气中的烃浓度,计算烃储存效率。银的存在显著改进HC捕集性能(表1)。
表1. 含有或不含银的新鲜状态的烃捕集器的烃储存效率
HC储存效率(%) | |
HC捕集器A | 54.3 |
HC捕集器C | 79.9 |
对这些烃捕集器进行如实施例5所述的老化,并测量烃储存效率。于800℃下老化和于900℃下老化后,银的益处较小,样品等同(表2)。
表2. 在水热老化后,含有或不含银的烃捕集器的烃储存效率
800℃ | 900℃ | |
HC捕集器A | 51.8 | 50.2 |
HC捕集器C | 68.9 | 53.8 |
实施例7 HC捕集器储存效率(氧)
通过将气体化学计量从贫转换到富并测量产生的CO2的量,使用合成废气测量氧储存。该测试给出被测试的烃捕集器的可用的氧储存的值。这些测量在200、250、300和350℃(预期旁路***中的烃捕集器通常操作的温度)下进行。这些测量对取自HC捕集器的1×3"芯进行。
表3. 用于测量氧储存容量的气体混合物
表4. 测量的HC捕集器B、C和D的氧储存容量,以mg/l烃捕集计
OSC,200℃ | OSC,250℃ | OSC,300℃ | OSC,350℃ | |
HC捕集器B | 11.1 | 20.7 | 27.3 | 58.7 |
HC捕集器C | 24.9 | 25.5 | 23.1 | 28.8 |
HC捕集器D | 108.8 | 125.5 | 174.0 | 243.4 |
仅含银的HC捕集器具有非常低水平的OSC(HC捕集器C)。仅含二氧化铈的HC捕集器在低温下具有低水平的OSC。对于HC捕集器B,OSC的水平在350℃下开始升高,但是对于在旁路***中的HC捕集器,这是在操作温度窗口的高端。含有银和二氧化铈两者的HC捕集器D具有高水平的氧储存,即使在200℃下。
实施例8 - HC效率和OSC容量之间的关系
HC捕集器D的水热老化导致OSC可测量的降低,同时HC捕集器的烃捕集效率降低至不足以使车辆满足相关排放法规的水平。
表5. 在新鲜状态下和在800和900℃下水热老化后,HC捕集器B、C和D在300℃下的烃储存效率和OSC
示于表5的HC捕集器B、C和D的烃效率和氧储存能力突显本发明的益处。
HC捕集器B含有二氧化铈源但是不含银。HC储存效率低,并且在低温下存在非常小的OSC。
HC捕集器C含有银但是不含二氧化铈源。新鲜的HC储存效率良好,且当HC捕集器老化时可清楚地看到劣化,但是OSC低,并且当HC捕集器老化时,OSC不存在显著变化。由于在该低温范围内OSC不存在显著变化,不能使用常规的机上诊断方法来确定HC捕集器的状况。
HC捕集器D含有二氧化铈源和银两者。HC储存像HC捕集器C的情况一样好,与HC捕集器B和C形成对照,HC捕集器D的OSC在低温下也非常高。当于800℃下水热老化时,HC捕集器D的OSC显著劣化,HC捕集器的HC储存效率也劣化。HC捕集器D的OSC的这个大的变化可通过常规机上诊断方法来测量。
使用现有的设备和技术,技术人员可设计和构建HC捕集***,并结合传感器装置和电子控制模块(ECM(无论单独的ECM还是通过现有OBD ECM的另外的程序化功能))。技术人员可使用常规的优化技术来得到具体的发动机的最佳结果。
Claims (14)
1.一种用于处理由火花-点火发动机产生的废气的***,所述***包含:
a. 烃捕集器(HC捕集器),其包含至少一个烃-吸收分子筛和牺牲性氧储存组件(OSC),其中所述OSC选为在低于烃-吸收材料的操作温度的温度下失去其氧储存容量的至少一部分;
b. 三路催化剂(TWC);
c. 流通导管,其用于引导废气的流动,其中所述流通导管与火花-点火发动机和TWC流体连通;和
d. 旁路导管,其具有与流通导管和HC捕集器流体连通的入口和与HC捕集器和流通导管流体连通的出口,其中所述入口布置在HC捕集器和TWC的上游,其中所述出口布置在HC捕集器的下游和TWC的上游。
2.权利要求1的***,其中所述至少一个烃-吸收分子筛选自以下框架类型编码:MFI、BEA、FAU、MOR、FER、ERI、LTL和CHA及其任何两种或更多种的混合物。
3.权利要求2的***,其中所述分子筛或每一个分子筛为铝硅酸盐沸石或SAPO。
4.权利要求1的***,其中所述牺牲性OSC在低于约800℃的操作温度下降解。
5.权利要求4的***,其中所述HC捕集器包含银。
6.权利要求5的***,其中所述牺牲性OSC包含铈源。
7.权利要求6的***,其中所述铈源选自负载的铈盐、块体二氧化铈(CeO2)或未经稳定的二氧化铈-氧化锆。
8.权利要求1-5中任一项的***,其中所述牺牲性OSC包含锰-二氧化钛。
9.权利要求1-5中任一项的***,其中所述牺牲性OSC包含锰-铝酸盐。
10.权利要求1-5中任一项的***,其中所述牺牲性OSC在小于约300℃下在新鲜催化剂中提供可检测的OSC活性。
11.权利要求1-5中任一项的***,所述***进一步包含用于测定HC捕集***的氧储存容量的传感器和电子控制模块,使得当收到来自传感器装置的指示氧储存容量的信号时,电子控制模块能确定是否牺牲性OSC已暴露于HC捕集器材料已降解的温度。
12.权利要求11的***,其中当所述废气的温度约为HC捕集器的最大操作温度时,所述HC捕集器可变换为相对于废气流动并线,并且当所述废气的温度小于HC捕集器的最大操作温度时,所述HC捕集器可变换为相对于废气流动离线。
13.权利要求1的***,所述***进一步包含布置在所述入口的下游和所述HC捕集器的上游的第二TWC。
14.一种用于HC捕集器的机上诊断(OBD)的方法,所述方法包括在HC捕集材料内结合牺牲性OSC,该牺牲性OSC的氧储存容量在最高约800℃的温度下降解,并通过测量HC捕集材料的氧储存容量来确定是否HC捕集器已暴露于HC捕集材料已降解并且不再对HC捕集有效的温度。
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GB0915326A GB2473215A (en) | 2009-09-03 | 2009-09-03 | HC trap system comprising an oxygen storage component material |
GB0915326.3 | 2009-09-03 | ||
PCT/IB2010/002598 WO2011027228A1 (en) | 2009-09-03 | 2010-09-03 | Improvements in emission control |
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US (1) | US8677739B2 (zh) |
EP (1) | EP2473720B1 (zh) |
JP (1) | JP5675818B2 (zh) |
KR (1) | KR101775993B1 (zh) |
CN (1) | CN102575546B (zh) |
BR (1) | BR112012004867B1 (zh) |
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US20120216508A1 (en) | 2012-08-30 |
RU2012112831A (ru) | 2013-10-10 |
CN102575546B (zh) | 2015-08-19 |
BR112012004867A2 (pt) | 2016-04-05 |
GB0915326D0 (en) | 2009-10-07 |
KR20120068010A (ko) | 2012-06-26 |
KR101775993B1 (ko) | 2017-09-19 |
BR112012004867B1 (pt) | 2020-07-07 |
EP2473720B1 (en) | 2016-11-02 |
JP5675818B2 (ja) | 2015-02-25 |
US8677739B2 (en) | 2014-03-25 |
GB2473215A (en) | 2011-03-09 |
JP2013504006A (ja) | 2013-02-04 |
RU2541486C2 (ru) | 2015-02-20 |
WO2011027228A1 (en) | 2011-03-10 |
EP2473720A1 (en) | 2012-07-11 |
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