CN104334255A - 三效催化剂体系 - Google Patents
三效催化剂体系 Download PDFInfo
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- CN104334255A CN104334255A CN201380027762.4A CN201380027762A CN104334255A CN 104334255 A CN104334255 A CN 104334255A CN 201380027762 A CN201380027762 A CN 201380027762A CN 104334255 A CN104334255 A CN 104334255A
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- way catalyst
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- 239000003054 catalyst Substances 0.000 title claims abstract description 154
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 47
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims abstract description 33
- 229910052684 Cerium Inorganic materials 0.000 claims abstract description 24
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims abstract description 23
- 239000010948 rhodium Substances 0.000 claims abstract description 20
- 229910052703 rhodium Inorganic materials 0.000 claims abstract description 18
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims abstract description 18
- 229910052763 palladium Inorganic materials 0.000 claims abstract description 16
- 239000000463 material Substances 0.000 claims abstract description 9
- 238000011144 upstream manufacturing Methods 0.000 claims abstract description 6
- 229910000510 noble metal Inorganic materials 0.000 claims description 17
- 230000003197 catalytic effect Effects 0.000 claims description 16
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 16
- 239000000203 mixture Substances 0.000 claims description 12
- 229910052779 Neodymium Inorganic materials 0.000 claims description 10
- QEFYFXOXNSNQGX-UHFFFAOYSA-N neodymium atom Chemical compound [Nd] QEFYFXOXNSNQGX-UHFFFAOYSA-N 0.000 claims description 9
- 229910052697 platinum Inorganic materials 0.000 claims description 7
- 229910052751 metal Inorganic materials 0.000 claims description 6
- 239000002184 metal Substances 0.000 claims description 6
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 5
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 claims description 5
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 4
- 239000001301 oxygen Substances 0.000 claims description 4
- 229910052760 oxygen Inorganic materials 0.000 claims description 4
- 241001466460 Alveolata Species 0.000 claims description 2
- 239000000969 carrier Substances 0.000 claims description 2
- PLDDOISOJJCEMH-UHFFFAOYSA-N neodymium(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Nd+3].[Nd+3] PLDDOISOJJCEMH-UHFFFAOYSA-N 0.000 claims description 2
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 abstract 1
- 229910052726 zirconium Inorganic materials 0.000 abstract 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 8
- 229910002091 carbon monoxide Inorganic materials 0.000 description 8
- 238000000576 coating method Methods 0.000 description 8
- 238000000034 method Methods 0.000 description 8
- 239000004215 Carbon black (E152) Substances 0.000 description 7
- 239000011248 coating agent Substances 0.000 description 7
- 239000007789 gas Substances 0.000 description 7
- 229930195733 hydrocarbon Natural products 0.000 description 7
- 150000002430 hydrocarbons Chemical class 0.000 description 7
- 239000000758 substrate Substances 0.000 description 6
- 238000012360 testing method Methods 0.000 description 6
- 238000001354 calcination Methods 0.000 description 5
- 239000003344 environmental pollutant Substances 0.000 description 5
- 238000000605 extraction Methods 0.000 description 5
- 231100000719 pollutant Toxicity 0.000 description 5
- 239000000725 suspension Substances 0.000 description 5
- 238000001035 drying Methods 0.000 description 4
- 239000000446 fuel Substances 0.000 description 4
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 229910004625 Ce—Zr Inorganic materials 0.000 description 3
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 3
- 239000007900 aqueous suspension Substances 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 238000002485 combustion reaction Methods 0.000 description 3
- 238000009472 formulation Methods 0.000 description 3
- UUCCCPNEFXQJEL-UHFFFAOYSA-L strontium dihydroxide Chemical compound [OH-].[OH-].[Sr+2] UUCCCPNEFXQJEL-UHFFFAOYSA-L 0.000 description 3
- 229910001866 strontium hydroxide Inorganic materials 0.000 description 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- RQPZNWPYLFFXCP-UHFFFAOYSA-L barium dihydroxide Chemical compound [OH-].[OH-].[Ba+2] RQPZNWPYLFFXCP-UHFFFAOYSA-L 0.000 description 2
- 229910001863 barium hydroxide Inorganic materials 0.000 description 2
- 229910052878 cordierite Inorganic materials 0.000 description 2
- 230000008021 deposition Effects 0.000 description 2
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 description 2
- 239000011159 matrix material Substances 0.000 description 2
- MMKQUGHLEMYQSG-UHFFFAOYSA-N oxygen(2-);praseodymium(3+) Chemical compound [O-2].[O-2].[O-2].[Pr+3].[Pr+3] MMKQUGHLEMYQSG-UHFFFAOYSA-N 0.000 description 2
- GPNDARIEYHPYAY-UHFFFAOYSA-N palladium(ii) nitrate Chemical compound [Pd+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O GPNDARIEYHPYAY-UHFFFAOYSA-N 0.000 description 2
- 229910003447 praseodymium oxide Inorganic materials 0.000 description 2
- 239000010970 precious metal Substances 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- 230000006641 stabilisation Effects 0.000 description 2
- IATRAKWUXMZMIY-UHFFFAOYSA-N strontium oxide Chemical compound [O-2].[Sr+2] IATRAKWUXMZMIY-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 150000000703 Cerium Chemical class 0.000 description 1
- 150000001206 Neodymium Chemical class 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- QVQLCTNNEUAWMS-UHFFFAOYSA-N barium oxide Inorganic materials [Ba]=O QVQLCTNNEUAWMS-UHFFFAOYSA-N 0.000 description 1
- CSSYLTMKCUORDA-UHFFFAOYSA-N barium(2+);oxygen(2-) Chemical compound [O-2].[Ba+2] CSSYLTMKCUORDA-UHFFFAOYSA-N 0.000 description 1
- 230000033228 biological regulation Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 238000011109 contamination Methods 0.000 description 1
- 238000011217 control strategy Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000000855 fermentation Methods 0.000 description 1
- 230000004151 fermentation Effects 0.000 description 1
- 238000007210 heterogeneous catalysis Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000005022 packaging material Substances 0.000 description 1
- 238000010422 painting Methods 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 239000013074 reference sample Substances 0.000 description 1
- 230000004044 response Effects 0.000 description 1
- VXNYVYJABGOSBX-UHFFFAOYSA-N rhodium(3+);trinitrate Chemical compound [Rh+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VXNYVYJABGOSBX-UHFFFAOYSA-N 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
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- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
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Abstract
本发明描述了一种三效催化剂体系,该三效催化剂体系包括在惰性催化剂载体上的一种第一三效催化剂和位于该第一三效催化剂上游的一种第二三效催化剂,该第一三效催化剂是一种双层催化剂、包括在惰性催化剂载体的一个第一层和施加到第一层上并与有待净化的排气直接接触的一个第二层,该第一层包括活性氧化铝、一种铈/锆混合氧化物和钯,该第二层包括活性氧化铝和铑且不含有铈及含铈材料。
Description
本发明描述了一种用于净化汽油发动机排气的三效催化剂体系。
在燃烧发动机领域中众所周知,燃料燃烧是不充分的并且产生污染物排放,这些污染物如未燃烧的碳氢化合物(HC),一氧化碳(CO),氮氧化物(NOX)和颗粒物(PM)。为了改进空气质量,设立了排放限制法规以实现来自固定应用和可移动来源的更低的污染物排放。对于像客车这种可移动来源,主要措施使得能够实现污染物排放的减少。改进燃料-空气混合作为主要措施产生了污染物的显著减少。然而,由于这些年更严格的法规,非均相催化剂的应用不可避免。
对于汽油发动机,所谓的三效催化剂(TWC)可去除HC,CO和NOX。TWC的最佳使用量是约λ=1+/-0.005,其中空气/燃料比等于14.56。超过这些值,排气是所谓的稀排气,并且CO和HC被催化氧化为二氧化碳和水。低于这个值,排气是所谓的富排气且用例如CO作为还原剂主要将NOX还原为N2。
在λ=1时,HC、CO和NOX可获得最佳的转化率。然而,汽油发动机在稍微的稀条件与稍微的富条件之间浮动的条件下工作。在纯粹的富条件下,烃的转化率迅速下降。为了扩展TWC的最佳工作,将以Ce混合氧化物形式的储氧材料(OSM)包含在该TWC的配方中。
对于这样的λ=1工作的汽油发动机,就所执行的排气系统而论有多种解决方案,这些排气系统涉及所包含的催化剂的数目和相对于发动机出口的位置。在一个紧密连接的发动机停机位置上的共用单块解决方案使用不同的基板、体积和贵金属负载量,以及均匀的或分区的催化剂类型。此外,在一个带有最少两块或更多块的排气系统情况下,所安装的催化剂例如在它们单独的体积、每一块的基板类型、贵金属负载和涂层类型(如均匀涂覆的或分区的催化剂)中有所区别。这些单独排气系统具有一个共同的功能界面,通过该发动机的λ控制而给定。该λ控制和该单独催化剂体系之间的相互作用需要进行优化以实现该排气系统的最好的排放特性。对于该催化剂体系的闭环控制行为,该选定的催化剂配方起着重要的作用。对于一个给定的λ控制策略,显而易见的是,优选的,一种对应的催化剂配方与该控制算法一起可产生最好的效果。另一方面,现代发动机管理系统提供了大范围的软件功能,这些软件功能允许以一种有意义的方式调节λ控制行为,以获得在优异排放性能方面催化剂体系的最好的响应。为了平衡优化的冲突范围,发展催化剂配方和体系是有效的,这些配方和体系能够以不损害排放性能,或甚至产生改进的情况下可减少应用复杂程度的方式解决这个问题。本发明的催化剂体系提供了一个如此折中的技术方案。
WO 2008/000449 A2描述了一个常规的双层三效催化剂。在这个发明中,第一层包含一种活性氧化铝和一种第一Ce/Zr混合氧化物,均用钯活化。第二层包含一种活性氧化铝和一种第二Ce/Zr混合氧化物,均用铑活化。该发明的特异性在于第一混合氧化物的Ce/Zr比高于第二混合氧化物的Ce/Zr比。
WO 2008/113445 A1也公开了一种双层三效催化剂,其中两层都包括活性氧化铝,Ce/Zr混合氧化物和钯。这些层的不同在于,第二层除了铂还包括铑且第一层混合氧化物的Ce/Zr比高于第二层混合氧化物的Ce/Zr比。
US 6,044,644和US 6,254,842公开了发动机附近的催化剂,该催化剂被设计用来减少在冷启动过程中来自汽油发动机的烃排放量。它包括用于一种TWC催化剂组合物中的类型的成分,只是实质上不含有氧化铈和氧化镨。
本发明提供了一种三效催化剂体系,包括
·在惰性催化剂载体上的一种第一三效催化剂,该催化剂是一种双层催化剂,包括
在该惰性催化剂载体上的一个第一层,该第一层包括活性氧化铝,一种铈/锆混合氧化物以及作为一种催化活性贵金属的钯,以及
一个第二层,该第二层被施加到第一层上并与有待净化的排气直接接触,包括活性氧化铝以及作为一种催化活性贵金属的铑,其中该第二层不含有铈和含铈材料且不包含除了铑以外的任何催化活性贵金属,和
·一种第二三效催化剂。
该第一三效催化剂的第一层除了钯以外,还可能包括作为附加的催化活性贵金属的铂和/或铑。在本发明的一个优选实施例中,除钯以外,铂也存在于第一层中。在本发明的另一个优选实施例中,除钯以外,第一层不包含其它任何催化活性贵金属。
该第一三效催化剂的催化活性贵金属用量是考虑到特定的操作要求并根据所希望的污染物转化率来选择的。典型地,钯是基于惰性催化剂载体的体积以0.1至15g/L的量使用。典型地铑的浓度是基于惰性催化剂载体的体积从0.01至1g/L。如果该第一三效催化剂的第一层中存在铂,其用量典型地是基于惰性催化剂载体的体积从0.01至1g/L。
该催化活性贵金属沉积到该催化剂的一种或多种其他成分上。例如,该第一层的催化活性贵金属可以沉积到活性氧化铝或者铈/锆混合氧化物或两者上。第一层和第二层的活性氧化铝通常通过掺杂基于氧化铝的总重量按重量计1%至10%,优选3%至6%且更优选3.5%至4.5%的氧化镧来稳定化。
用于第一三效催化剂的第一层中的铈/锆混合氧化物的特征为氧化铈与氧化锆的重量比。这样的重量比可以在广泛的界限内变化,且取决于催化剂预期解决的特定技术任务。典型地氧化铈与氧化锆的重量比是从0.1至1.2且优选从0.8至1.2。该铈/锆混合氧化物优选以基于惰性催化剂载体的体积40至60 g/L的量使用。
为了本发明的目的,术语“不包含铈和含铈材料”意思是第一三效催化剂的第二层不包含显著量的铈或含铈材料。然而,这个术语不意味着本发明的催化剂的第二层不能包含小量值的铈或含铈材料,它可能以杂质的形式存在或可能已经从第一层迁移到第二层。
在本发明的一个优选实施例中,该第一三效催化剂的第二层包括一种钕/锆混合氧化物。在此混合氧化物中氧化钕与氧化锆的重量比优选是从0.2至0.5。该钕/锆混合氧化物优选基于惰性催化剂载体的体积以50至80g/L的量使用。
在钕/锆混合氧化物存在于第一三效催化剂的第二层中的情况下,铑可以沉积到活性氧化铝或者钕/锆混合氧化物或两者上。优选地,铑沉积到活性氧化铝和钕/锆混合氧化物两者上。
在本发明的另一个实施例中,在第一三效催化剂的第二层完全覆盖第一层。在这种情况下,第一层不直接与有待净化的排气接触。
在本发明的一个附加的实施例中,本发明的三效催化剂体系的第一三效催化剂包括一个在惰性催化剂载体与第一层之间的中间层。典型地,所述中间层包括活性氧化铝且不含有铂族金属。中间层优选地基于惰性催化剂载体的体积以40至80g/L的量使用。
本发明的三效催化剂体系的第二三效催化剂通常是根据现有技术的一种常规的三效催化剂。例如在WO 2008/000449 A2和WO 2008/113445 A1中描述了适合的实例。因此,第二三效催化剂优选地包括在一种大比表面积、耐高温的氧化物载体上的一种或多种铂族金属,如铂、钯和铑。一种优选的大比表面积、耐高温的氧化物载体是大比表面积的氧化铝,该氧化铝特别地优选通过增加基于氧化铝的总重量按重量计1%至10%,优选3%至6%且更优选3.5%至4.5%的氧化镧来稳定化。此外,该第二三效催化剂优选地包括一种或多种储氧成分。优选的储氧成分是氧化镨、氧化铈和如Ce/Zr混合氧化物的含氧化铈材料。如第一三效催化剂,第二三效催化剂优选地负载在一种惰性催化剂载体上。在所述的载体上的该第二三效催化剂以包含上文所提及的所有成分的一个层的形式存在,或以关于铂族金属和/或储氧成分以不同于彼此的两个或甚至更多层的形式存在。
在本发明的一个特别优选的实施例中,第一三效催化剂不同于第二三效催化剂。
优选的用于第一和第二三效催化剂的惰性催化剂载体是具有体积V的陶瓷或金属的单块,该单块具有用于内燃发动机排气的平行流动通道。这些流动通道的壁表面用根据本发明的三效催化剂涂覆。优选地,该惰性催化剂载体是一种具有蜂窝状结构的流通式单块。
在本发明的一个实施例中,该第一三效催化剂和该第二三效催化剂负载在不同的惰性催化剂载体上。换句话说,第一三效催化剂和第二三效催化剂负载在不同的块上。
在本发明的另一个实施例中,该第一三效催化剂和该第二三效催化剂负载在相同的惰性催化剂载体上。换句话说,第一三效催化剂和第二三效催化剂形成一种所谓的分区催化剂,其中该第一三效催化剂位于该载体的下游侧且该第二三效催化剂位于该载体的上游侧。
本发明的三效催化剂体系可通过已知的方法来制造。关于第一三效催化剂,这些层优选地是通过载体涂覆(wash-coating)过程涂覆在载体上。相应地,将预期用于特定层的固体悬浮在水中。在第一层的情况下,这些是活性氧化铝和一种铈/锆混合氧化物。从可溶于水的贵金属盐出发,钯和任选地铂和/或铑沉积到这些材料上。对于钯的情况,优选使用在US 6,103,660中描述的方法中的硝酸钯,用氢氧化钡或氢氧化锶作为基体。以此获得的悬浮液可以直接用于涂覆该催化剂载体。随后将所施加的层干燥和任选地煅烧。
使用氢氧化钡或氢氧化锶作为基体使硝酸钯沉淀,导致在最后的煅烧之后,剩余氧化钡或氧化锶,它们已经沉积到活性氧化铝和铈/锆混合氧化物的表面上。在第一三效催化剂的第一层中使用了催化活性贵金属混合物的情况下,有可能在一个操作中或相继地在多个不同的操作中完成所有的金属混合物的沉积。
在其后,施加第二涂层。为此,将活性氧化铝和任选的钕/锆混合氧化物悬浮于水中,并且将铑沉积在其上。这可以通过供应硝酸铑实现。最后,将负载第一和第二层的载体干燥和煅烧然后就准备好使用。
替代于所描述的程序,该催化活性贵金属也可以分开地沉积到催化剂的任何固体成分上。只有在其后,例如,钯活化的氧化铝和钯活化的铈/锆混合氧化物一起悬浮在水中并施加到催化剂载体上。这样一个程序,一方面使在氧化铝上的催化活性贵金属的浓度能够以一种受控的方式确立,另一发面使例如铈/锆混合氧化物或钕/锆混合氧化物的浓度能够以一种受控的方式确立。为了贵金属向氧化铝和锆混合氧化物上的分开的沉积,给予优选的是使用在EP 957064中所描述的方法。
在本发明的三效催化剂体系包括两个块的情况下,将由此获得的涂覆的载体与一个第二块组合,该第二块携带第二三效催化剂且也优选地已经通过载体涂覆过程被制造。在本发明的三效催化剂体系仅包括一个块的情况下,第一三效催化剂通过如上所述的一种载体涂覆方法被施加到该载体上,然而不同之处是,第一三效催化剂只是被施加到该载体总长度的一部分上。实际上,第一三效催化剂开始于该载体的一端(一旦该载体在使用中,这将是下游端)到一个小于该载体总长度的给定的长度上被施加。第二三效催化剂将类似地被施加,然而开始于该载体的另一端(一旦该载体在使用中,这将是上游端)且也结束在一个小于该载体总长度的给定的长度上。若该载体的总长度是L,包括第一三效催化剂区的长度是a且包括第二三效催化剂区的长度是b,优选地L=a+b。
本发明的三效催化剂体系对清洁配备汽油发动机的机动车辆的排气是合适的,并且可以为了这个目的使用技术人员已知的方法。因此,本发明进一步提供了本发明的三效催化剂体系用于清洁配备汽油发动机的机动车的排气的用途,其中该第二三效催化剂位于该第一三效催化剂的上游。
实例
对于本发明的测试,使用的圆形堇青石基板直径101.6mm、长度76.2mm。泡孔密度是600cpsi且壁厚是4.3mil。
对比实例:
将根据WO 2008/000449 A2的两个完全相同的双层三效催化剂组合成一个三效催化剂体系,且被用作参比样品。每个双层三效催化剂根据所述公开中描述的配方如下地制备:
a)对于第一层,水性悬浮物通过将一种氧化镧稳定的氧化铝与一种第一Ce-Zr混合氧化物混合来制备,该氧化镧稳定的氧化铝含有3wt.%的La2O3且具有140m2/g的比表面积,该第一Ce-Zr混合氧化物具有50%的ZrO2含量,且氢氧化锶作为碱性成分。将Pd(NO3)2作为贵金属前驱体使用并沉积到所有氧化物上。在最终完成该悬浮物之后,将原堇青石基板用第一层涂覆,随后的是一个干燥步骤。煅烧之后,第一层的组成是:
b)对于第二层,制备了包含氧化镧稳定的氧化铝(3wt.%的La2O3,比表面积等于140m2/g)和具有70%的ZrO2含量的第二Ce-Zr混合氧化物的水性悬浮物。将Rh(NO3)2水溶液注射到悬浮物中。将第二层涂覆到第一层的顶部上。在干燥和煅烧步骤之后,第二层的组成是:
70g/L La稳定的氧化铝
65g/L 第二CeZr混合氧化物
0.11g/L 铑(在所有成分上)
以此获得的两个涂层基板相组合以形成一种体系。在下面描述的测试中所得的催化剂体系称为CC1。
实例1:
为了获得一种本发明的三效催化剂体系,CC1的上游基板保持不变,而下游基板生产如下:
a)与堇青石基板相接触的第一层精确地按照对比实例中的步骤a)所描述地制备并且因此具有相同的组成。
b)对于第二层,制备含有氧化镧稳定的氧化铝(3wt.%的La2O3,比表面积等于140m2/g)并具有73%ZrO2含量的Zr/Nd混合氧化物的水性悬浮物。将Rh(NO3)2水溶液注射到悬浮物中。将第二层涂覆到第一层的顶部上。在干燥和煅烧步骤之后,第二层的组成是:
66g/L La稳定的氧化铝
68g/L Zr/Nd混合氧化物
0.11g/L 铑(在所有成分上)
在下面描述的测试中所得的催化剂体系称为C1。
在一个2L的发动机上,950℃的入口温度下,使用联邦试验规程(FTP)75测试循环,在严重的停止供油(fuel cut)老化之后,将对比实例(CC1)和实例1(C1)的催化剂进行比较。该发动机的λ控制系统包含一个位于发动机出口的大量程传感器和一个安装在该对应催化剂体系的两块后的跃迁传感器。两种催化剂体系在λ控制软件上用相同的配置比较。λ控制设置与在车辆的系列应用中相同。通常来说,该FTP 75测试循环包括一个相比于欧洲NEDC排放测试循环动态得多的驾驶行为,因此特别地该催化剂体系的NOX排放性能将受到大得多的压力且λ控制与催化剂体系间的相互作用的质量变得更明显。这更好的允许评估不同催化剂体系的预热转换效率,这导致在所调研的系统之间一个更大的差别性。
获得以下结果:
NOX:
THC:
CO:
因此,关于THC和CO,虽然CC1和C1性能类似,但关于NOX,本发明体系C1性能更出色。
Claims (15)
1.三效催化剂体系,包括
·在一种惰性催化剂载体上的一种第一三效催化剂,该第一三效催化剂是一种双层催化剂,包括
在该惰性催化剂载体上的一个第一层,该第一层包括活性氧化铝,一种铈/锆混合氧化物以及作为一种催化活性贵金属的钯以及
一个第二层,该第二层被施加到第一层上并与有待净化的排气直接接触,包括活性氧化铝以及作为一种催化活性贵金属的铑,其中该第二层不含有铈和含铈材料且不包含除了铑以外的任何催化活性贵金属,和
·一种第二三效催化剂。
2.根据权利要求1所述的三效催化剂体系,其特征在于在该第一三效催化剂的第一层中除了钯以外,还使用铂或铑或其混合物作为催化活性贵金属。
3.根据权利要求1所述的三效催化剂体系,其特征在于该第一三效催化剂的第一层不包含除钯以外的任何催化活性贵金属。
4.根据权利要求1至3中的一项或多项所述的三效催化剂体系,其特征在于在该第一三效催化剂的第一层的铈/锆混合氧化物中氧化铈与氧化锆的重量比为从0.1至1.2。
5.根据权利要求1至4中的一项或多项所述的三效催化剂体系,其特征在于该第一三效催化剂的第二层包括一种钕/锆混合氧化物。
6.根据权利要求5所述的三效催化剂体系,其特征在于在该第一三效催化剂的第一层的钕/锆混合氧化物中氧化钕与氧化锆的重量比为从0.2至0.5。
7.根据权利要求5所述的三效催化剂体系,其特征在于该第一三效催化剂的该第二层中铑沉积到活性氧化铝和钕/锆混合氧化物两者上。
8.根据权利要求1至3中的一项或多项所述的三效催化剂体系,其特征在于该第一三效催化剂的第二层完全覆盖该第一三效催化剂的第一层。
9.根据权利要求1至8中的一项或多项所述的三效催化剂体系,其特征在于该第一三效催化剂的惰性催化剂载体是一种具有蜂窝状结构的流通式单块。
10.根据权利要求1至9中的一项或多项所述的三效催化剂体系,其特征在于该第二三效催化剂包括在一种大比表面积、耐高温的氧化物载体上的一种或多种铂族金属。
11.根据权利要求1至10中的一项或多项所述的三效催化剂体系,其特征在于该第二三效催化剂包括一种或多种储氧成分。
12.根据权利要求1至11中的一项或多项所述的三效催化剂体系,其特征在于该第一三效催化剂不同于该第二三效催化剂。
13.根据权利要求1至12中的一项或多项所述的三效催化剂体系,其特征在于该第一三效催化剂和该第二三效催化剂负载在不同的惰性催化剂载体上。
14.根据权利要求1至12中的一项或多项所述的三效催化剂体系,其特征在于该第一三效催化剂和该第二三效催化剂负载在相同的惰性催化剂载体上。
15.根据权利要求1至14中的一项或多项所述的三效催化剂体系用于清洁配备汽油发动机的机动车辆的排气的用途,其中该第二三效催化剂位于该第一三效催化剂的上游。
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EP2858738A1 (en) | 2015-04-15 |
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US9522360B2 (en) | 2016-12-20 |
EP2858738B1 (en) | 2019-11-20 |
US20150125371A1 (en) | 2015-05-07 |
JP2015525123A (ja) | 2015-09-03 |
WO2013182303A1 (en) | 2013-12-12 |
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