CN101970820B - 排放控制的改进 - Google Patents
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- F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
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- F01N3/2803—Construction of catalytic reactors characterised by structure, by material or by manufacturing of catalyst support
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Abstract
一种以天然气作为燃料的贫燃柴油发动机，包括排气系统，排气系统包括氧化催化剂。发动机可以被用于汽车应用，例如给车辆提供动力，或者可以是用于发电的固定发动机。
Description
技术领域
本发明涉及排放控制的改进。更具体地，本发明尤其涉及装有催化式排放控制系统的以天然气作为燃料的内燃机，通常用于车辆应用，不过也可以被用于处理来自用于发电的固定发动机的排放。
背景技术
在本说明书和权利要求书中，术语“柴油发动机”将被用于表示压缩点火式内燃机。
在重型柴油发动机中有倾向于使用压缩天然气的趋势，至少有部分原因是出于这样的发动机在废气排放方面要比液体柴油作为燃料的发动机“更加清洁”的认知。本发明既可以被应用于新构造的发动机，也可以被应用于经过改装从而用天然气运行而不再用液体柴油燃料运行的柴油发动机。通常天然气可以作为压缩天然气(CNG)被存储，或者如果合适的话也可以作为液化天然气(LNG)被存储。
术语“天然气”包括从矿源例如天然气井获得的含有甲烷体积超过30％的气体，以及与来自生物质气化、煤气化过程、垃圾填埋场的其他高级烃有关的气体，或者是通过碳氧化物的氢化和其他的甲烷形成过程而生产出的气体。
甲烷自身以及天然气的十六烷值(CN)通常对于单独作为燃料在未经改装的柴油发动机内使用来说都是过低的。天然气例如可以与为天然气燃烧提供足够温度的柴油燃料点燃喷射结合使用。天然气可以在已经过改装的柴油发动机内使用以在一个或多个气缸内用火花塞点燃天然气。其他的发动机改装例如可以包括改变压缩比以在用天然气运行时优化性能。
用天然气运行的发动机可以在两种模式中的至少一种模式下工作；化学计量地使用与天然气的燃烧量处于化学平衡的氧气，并且通常这将对应于大约为17的空燃比，远远高于液态烃。然后可以用类似于在常规的汽油发动机上使用的“三元催化剂”来控制废气排放。第二种工作模式是其中氧气相对于天然气的燃烧量是过量的。这样的贫燃操作具有性能上的好处，并且通常被用于经过改装以用天然气运行的柴油发动机中。
用于以天然气作为燃料的贫燃柴油发动机的常规排放控制系统具有氧化催化剂，带有或者不带有附加组件，例如形式为催化烟灰过滤器的颗粒物捕集器，还具有SCR催化剂联同还原剂喷射系统。氧化催化剂位于排放系统内留有空间的位置。所有的现代重型柴油发动机均为涡轮增压式，并且涡轮增压器被设置为靠近发动机排气歧管，不仅是因为涡轮增压器单元必须由排气提供动力而且同时还要压缩进气。
在以天然气作为燃料的发动机的情况下，我们相信一种新的设置方式将会是有利的。甲烷与其他的高级烃相比需要高温用于催化氧化，催化氧化依赖于特定条件例如存在的甲烷量、流速等。温度通常为大约450℃或更高。尽管负载下运行的重型柴油发动机生成的废气温度在600℃左右，但是在部分负载状态下将会明显低于这种温度，并且涡轮增压器通常都是大尺寸并且同时会吸收能量以给压缩机提供动力从而明显地冷却废气。因此，涡轮增压器的安装通常会造成废气温度下降100℃或更多，这取决于工作状态。由于氧化催化剂通常被设置在与涡轮增压器相距一米或更远的位置，因此废气在排气管内会进一步冷却，并且结果是甲烷在氧化催化剂上经常只有很低的转化率。
排放标准的最初目的是减少臭氧形成，由于以此为基础的历史原因，目前在美国并未指定甲烷排放的标准。因此，还没有对减少来自发动机的甲烷排放或者提高甲烷的催化转化率的需求。尽管如此，但甲烷仍是一种重要的“温室气体”并且也希望能够将甲烷排放最小化。
US 2005/0229900公开了一种用于内燃机例如柴油、汽油或天然气发动机的排气系统以及就地生成氨以用于减少排气中的某些排放组分的方法。氨由产生于第一气缸组的富燃废气催化生成。氧化催化剂可以位于涡轮增压器上游，用于在贫燃废气中将NO氧化为NO2以由第二气缸组生成大约为1∶1的NO∶NO2混合物。
CA 2285780公开了一种发电方法和天然气发电系统，也就是固定发电源。该系统包括位于发动机和涡轮增压器之间的催化转化器。JP 11-350942公开了一种类似的系统。
SAE 2001-01-0189公开了一种涡轮增压器前端的氧化催化剂，用于处理来自于车辆柴油发动机的烃类和一氧化碳。
发明内容
本发明的目的在于改进贫燃的以天然气作为燃料的柴油发动机的排放控制以及在总体上改善环境。
根据一个方面，本发明提供了一种以天然气作为燃料的贫燃柴油发动机，可选地是重型发动机，包括排气系统，排气系统包括氧化催化剂。发动机可以被用于在处理废气时使用，废气来自于汽车应用，例如车辆应用，譬如用于卡车、公共汽车等的重型柴油发动机，或者可以被用于在处理用于发电的固定发动机时使用。
在一个具体的实施方案中，排气系统包括排气驱动的涡轮增压器，其中氧化催化剂位于发动机和涡轮增压器之间。在一个实施方案中，氧化催化剂位于每一个气缸的排气歧管内。在另一个实施方案中，氧化催化剂刚好位于涡轮增压器前方，例如位于涡轮增压器壳体的入口侧内。
在实施方案中，氧化催化剂包括至少一种贵金属，也就是金、银和铂族金属：钌、铑、钯、锇、铱和铂。例如，至少一种贵金属可以从由铂、钯和金包括其组合构成的组中选出。在一个优选实施方案中，氧化催化剂中的贵金属由钯和金的组合构成，可选地是钯和金的合金。
在某些实施方案中，氧化催化剂包括钯和金的组合，其中至少一部分可以作为合金存在。出于多种原因，该实施方案是特别有利的。首先，从实施例中能够看出Pd:Au与可比较的仅含Pd的催化剂相比对于处理甲烷而言更有活性。第二，仅含钯的催化剂的活性可能会由于燃料中存在的硫而中毒。但是，正如实施例中所指出的，Pd:Au催化剂与仅含Pd的催化剂相比更容易脱硫。而且，在Pd:Au催化剂位于涡轮增压器前端的实施方案中，催化剂可以被暴露在更高的废气温度下，这就能够降低催化剂在第一位置被硫化的可能性和/或将催化剂暴露于能够驱散在生成比较低温废气的驱动状态期间被吸附在催化剂上的所有硫的废气温度下。Pd:Au催化剂还具有相对较高的耐热性。
根据另一个方面，本发明提供了一种车辆，可选地是重型车辆，包括了根据本发明的发动机。
在另一个方面中，本发明提供了一种改进来自以天然气作为燃料的贫燃柴油发动机的甲烷排放的方法，包括输送来自于发动机的废气通过能在废气温度下有效氧化甲烷的氧化催化剂。
在一个具体的实施方案中，该方法提供了将由氧化催化剂处理过的废气输送到涡轮增压器内的步骤。
尽管本发明中在涡轮增压器前端的实施方案需要对系统组分有更好的“填装”，但是该问题可以改善，原因在于涡轮增压器上游的氧化催化剂的体积与常规的位于涡轮增压器下游的大体积的氧化催化剂相比能够被明显减小。可以预见的是上游的氧化催化剂可以与下游的氧化催化剂结合使用。在本发明中，氧化催化剂被暴露于惊人的废气高温以及脉动的废气压力之下，并且能够表现出针对甲烷的高转化效率。
可以预见的是尽管废气在通过氧化催化剂之后会有一定的少量压力损失，但是，由烃类氧化造成的放热将通过升高废气温度以及进入涡轮增压器的废气中的内能而至少部分地加以补偿。
根据具体发动机的特性以及有效的排放标准，排放控制系统可以包括附加组件。具体地，我们想要提及的是颗粒过滤器和催化式颗粒过滤器(具有被动或主动的再生控制系统)、NOX捕集器或NOX转化催化剂以及选择性催化还原(SCR)转化催化剂和还原剂喷射装置。附加组件例如氨破坏催化剂可以设置在SCR催化剂的下游。推荐使用还原剂喷射的电子控制。
用于在本发明中使用的合适的氧化催化剂被加有铂或钯或金或其混合物(10到250g/cu ft)以及流通式载体上携带的耐火氧化物。载体优选是金属的，但是合适的耐火陶瓷载体也可以考虑。常规的催化剂沉积方法和催化剂结构均可使用。
附图说明
为了能够更便于理解本发明，仅作为说明并参照附图给出以下的实施例，在附图中：
图1是示出了一定范围内的钯、金以及钯/金催化剂在硫酸化之前和之后的甲烷氧化活性的示意图；以及
图2是示出了AuPd催化剂在从30℃加热到850℃期间的XRD的示意图。
具体实施方式
实施例
催化剂制备和测试过程
以Pd:Au在0:1到1:0之间的原子组成分布在Al2O3上的一系列Pd-Au催化剂按如下所述进行制备：向含有颗粒状氧化铝载体的硝酸钯和HAuCl4的含水混合物中加入碱以将金作为Au0水解并沉积到载体上。经过适当的时段之后过滤浆料，滤液被冲洗以去除氯离子，并且随后煅烧经过干燥的材料。根据该工艺制备的催化剂在本文中被称作“新鲜的”催化剂。
在微型反应器内测试催化剂，微型反应器具有垂直的10mm直径的不锈钢反应管以及保留在不锈钢玻璃料上的催化剂粉末(0.4g)。气流(2升/分钟)向下，并且进入和排出的气体组成用各种自动分析设备测定，由此用常规方法来计算转化率。催化剂床温通过包围反应管的烘箱恒温地保持在设定温度，或者从110℃开始以10℃/分钟的速率上升至预定的测试温度。通过在300℃下输送含有氮气、水蒸汽和100-150ppm的二氧化硫(SO2)的气体混合物一定时间，例如将催化剂暴露给范围在15-400mg硫/g催化剂范围内的预定量的硫，而将催化剂硫酸化。随后在从110℃到500℃的温度下测试被硫酸化的催化剂的氧化活性。在达到500℃时，将催化剂保持在该温度下20分钟以模拟此时一部分硫可能会从催化剂中释放的操作。然后冷却至110℃并重复活性测试过程。
实施例1
图1示出了一定范围内的钯、金以及钯/金催化剂在硫酸化之前和之后的甲烷氧化活性。测试气体包括一氧化碳(1000ppm)、氧化氮(200ppm)、二氧化硫(2ppm)、甲烷(900ppm)、二氧化碳(4.5％)、水蒸汽(4.5％)、氧气(8％)以及余量的氮气。这些结果证实了钯催化剂对于甲烷氧化具有良好的活性(曲线A，2％Pd)。相比之下，仅含金的催化剂具有不良的甲烷氧化活性(曲线B，0.5％Au)。令人吃惊地，将金加入钯催化剂明显增强了甲烷氧化性能(曲线C，2％Pd+0.5％Au)。
在硫酸化后，钯催化剂表现出活性的明显损失(曲线D，2％Pd)，而含有钯和金的催化剂则表现出更大的活性损失(曲线E，2％Pd+0.5％Au)。因此未硫酸化的钯/金催化剂具有极佳的活性，而在被硫酸化后则性能不良。含有相对高含量金的催化剂(B，0.5％Pd和1％Au)在新鲜时也具有这样的不良活性，而未在被硫酸化时进行测试。
实施例2
本实施例示出了钯/金催化剂在比仅含钯的催化剂低得多的温度下即可被脱硫并再活化以用于氧化反应，并且这也是在与存在于以天然气作为燃料的发动机上的涡轮增压器之前的那些相比更低的温度下进行的，因此那里进行的脱硫连续有效，从而保持高催化性能。如上所述来制备和测试催化剂。测试气体包括一氧化碳(1000ppm)、氧化氮(200ppm)、二氧化硫(2ppm)、丙烯，(900ppm作为C1)、二氧化碳(4.5％)、水蒸汽(4.5％)、氧气(12％)以及余量的氮气。所得测试结果在表1中给出，其形式为实现80％的一氧化碳转化(COT80)和50％的烃类转化(HCT50)所需的温度。
表1.未硫酸化、硫酸化以及在500℃处理了20分钟之后的硫酸化催化剂的测试结果。在测试之前催化剂在750℃下老化48小时。
这些结果表明向钯催化剂中加入金降低了将硫酸化的催化剂再活化以用于氧化反应所处的温度，并且这种效果可能是很显著的。在测试之前，通过在750℃下加热48小时来老化这些催化剂，并且我们相信通过使金和钯构成合金可以至少部分地造成钯/金配方再活化的增强。X射线衍射证实了合金的形成。金和钯具有几乎完美的互溶性并且对应的晶格膨胀与形成的合金组成线性相关。
图2示出了从金(Ⅲ)和钯(Ⅲ)的2θ区域内的X射线反射。在催化剂样本被从30℃加热到850℃时，图2中这两个被标记的反射之间的合金相反射在强度上增加，证实了该相的存在。
Claims (10)
1.一种以天然气作为燃料的贫燃压缩点火式内燃机，包括排气系统，排气系统包括有效用于在废气温度下氧化甲烷的氧化催化剂，其中该氧化催化剂是钯和金的组合。
2.如权利要求1所述的发动机，其中排气系统包括排气驱动的涡轮增压器，并且其中氧化催化剂位于发动机和涡轮增压器之间。
3.如权利要求2所述的发动机，其中氧化催化剂位于排气歧管内。
4.如权利要求3所述的发动机，其中发动机具有多个气缸并且每一个气缸都在其排气歧管内具有氧化催化剂。
5.如权利要求2所述的发动机，其中氧化催化剂位于涡轮增压器的废气入口内。
6.如前述权利要求任一项所述的发动机，其中至少一部分钯和金作为合金存在。
7.一种车辆，包括根据前述任意一项权利要求所述的发动机。
8.一种根据权利要求1至6中的任意一项所述的用于发电的固定发动机。
9.一种改进来自以天然气作为燃料的贫燃柴油发动机的甲烷排放的方法，包括输送来自于发动机的废气通过有效用于在废气温度下氧化甲烷的氧化催化剂，其中该氧化催化剂是钯和金的组合。
10.如权利要求9所述的方法，包括将由氧化催化剂处理过的废气输送到涡轮增压器内。
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- 2009-02-27 KR KR1020107021421A patent/KR20100125358A/ko not_active IP Right Cessation
- 2009-02-27 US US12/919,822 patent/US20110113774A1/en not_active Abandoned
- 2009-02-27 EP EP09715321A patent/EP2257698A1/en not_active Withdrawn
- 2009-02-27 CN CN200980106930.2A patent/CN101970820B/zh not_active Expired - Fee Related
- 2009-02-27 JP JP2010548179A patent/JP5722048B2/ja not_active Expired - Fee Related
- 2009-02-27 BR BRPI0907817-7A patent/BRPI0907817A2/pt not_active Application Discontinuation
- 2009-02-27 WO PCT/GB2009/000563 patent/WO2009106849A1/en active Application Filing
- 2009-02-27 GB GB1013872.5A patent/GB2471582B/en not_active Expired - Fee Related
- 2009-02-27 DE DE112009000423T patent/DE112009000423T5/de not_active Withdrawn
- 2009-02-27 RU RU2010139652/06A patent/RU2505686C2/ru not_active IP Right Cessation
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB2396123A (en) * | 2002-12-11 | 2004-06-16 | Clean Air Partners Inc | Heat retention of an oxidation catalyst of a multi-fuel engine |
Also Published As
| Publication number | Publication date |
|---|---|
| BRPI0907817A2 (pt) | 2015-07-21 |
| US20110113774A1 (en) | 2011-05-19 |
| EP2257698A1 (en) | 2010-12-08 |
| WO2009106849A1 (en) | 2009-09-03 |
| JP2011514950A (ja) | 2011-05-12 |
| GB2471582B (en) | 2012-08-22 |
| CN101970820A (zh) | 2011-02-09 |
| GB201013872D0 (en) | 2010-09-29 |
| RU2505686C2 (ru) | 2014-01-27 |
| JP5722048B2 (ja) | 2015-05-20 |
| GB0803670D0 (en) | 2008-04-09 |
| GB2471582A (en) | 2011-01-05 |
| KR20100125358A (ko) | 2010-11-30 |
| RU2010139652A (ru) | 2012-04-10 |
| DE112009000423T5 (de) | 2010-12-30 |
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