CN112135685A - 三元催化剂 - Google Patents
三元催化剂 Download PDFInfo
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- CN112135685A CN112135685A CN201980033399.4A CN201980033399A CN112135685A CN 112135685 A CN112135685 A CN 112135685A CN 201980033399 A CN201980033399 A CN 201980033399A CN 112135685 A CN112135685 A CN 112135685A
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- catalyst
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- 239000003054 catalyst Substances 0.000 title claims abstract description 94
- 229910052751 metal Inorganic materials 0.000 claims abstract description 82
- 239000002184 metal Substances 0.000 claims abstract description 82
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims abstract description 78
- 239000000758 substrate Substances 0.000 claims abstract description 63
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 76
- 229910052763 palladium Inorganic materials 0.000 claims description 34
- 239000010948 rhodium Substances 0.000 claims description 29
- 229910052703 rhodium Inorganic materials 0.000 claims description 23
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims description 23
- 238000000034 method Methods 0.000 claims description 16
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 11
- 239000000463 material Substances 0.000 claims description 11
- 239000000203 mixture Substances 0.000 claims description 10
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 8
- 239000011248 coating agent Substances 0.000 claims description 8
- 238000000576 coating method Methods 0.000 claims description 8
- 238000002485 combustion reaction Methods 0.000 claims description 8
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims description 6
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 6
- 229910052697 platinum Inorganic materials 0.000 claims description 6
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 4
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 claims description 4
- 150000001875 compounds Chemical class 0.000 claims description 4
- 230000008569 process Effects 0.000 claims description 4
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 claims description 3
- 239000000395 magnesium oxide Substances 0.000 claims description 3
- 239000000377 silicon dioxide Substances 0.000 claims description 3
- 239000007864 aqueous solution Substances 0.000 claims description 2
- 239000000725 suspension Substances 0.000 claims description 2
- 238000004519 manufacturing process Methods 0.000 claims 1
- 239000007789 gas Substances 0.000 description 18
- 238000011068 loading method Methods 0.000 description 13
- -1 platinum group metals Chemical class 0.000 description 11
- 239000002002 slurry Substances 0.000 description 10
- 238000012360 testing method Methods 0.000 description 10
- 239000000446 fuel Substances 0.000 description 9
- 229930195733 hydrocarbon Natural products 0.000 description 9
- 150000002430 hydrocarbons Chemical class 0.000 description 9
- 231100000572 poisoning Toxicity 0.000 description 8
- 230000000607 poisoning effect Effects 0.000 description 8
- 239000000243 solution Substances 0.000 description 8
- 230000032683 aging Effects 0.000 description 6
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 5
- 229910002091 carbon monoxide Inorganic materials 0.000 description 5
- 230000000052 comparative effect Effects 0.000 description 5
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 4
- 230000008901 benefit Effects 0.000 description 4
- 238000001354 calcination Methods 0.000 description 4
- 239000003344 environmental pollutant Substances 0.000 description 4
- 230000007246 mechanism Effects 0.000 description 4
- 231100000719 pollutant Toxicity 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 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 3
- 239000010705 motor oil Substances 0.000 description 3
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 239000013618 particulate matter Substances 0.000 description 3
- 239000002574 poison Substances 0.000 description 3
- 231100000614 poison Toxicity 0.000 description 3
- 239000002904 solvent Substances 0.000 description 3
- 238000003756 stirring Methods 0.000 description 3
- 238000013316 zoning Methods 0.000 description 3
- ANHQLUBMNSSPBV-UHFFFAOYSA-N 4h-pyrido[3,2-b][1,4]oxazin-3-one Chemical group C1=CN=C2NC(=O)COC2=C1 ANHQLUBMNSSPBV-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 101150030566 CCS1 gene Proteins 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- 229910052684 Cerium Inorganic materials 0.000 description 2
- 229910004625 Ce—Zr Inorganic materials 0.000 description 2
- 101100332461 Coffea arabica DXMT2 gene Proteins 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 2
- 101100341123 Saccharomyces cerevisiae (strain ATCC 204508 / S288c) IRA2 gene Proteins 0.000 description 2
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- TZCXTZWJZNENPQ-UHFFFAOYSA-L barium sulfate Inorganic materials [Ba+2].[O-]S([O-])(=O)=O TZCXTZWJZNENPQ-UHFFFAOYSA-L 0.000 description 2
- 101150104736 ccsB gene Proteins 0.000 description 2
- ZMIGMASIKSOYAM-UHFFFAOYSA-N cerium Chemical compound [Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce] ZMIGMASIKSOYAM-UHFFFAOYSA-N 0.000 description 2
- RCFVMJKOEJFGTM-UHFFFAOYSA-N cerium zirconium Chemical class [Zr].[Ce] RCFVMJKOEJFGTM-UHFFFAOYSA-N 0.000 description 2
- 239000003638 chemical reducing agent Substances 0.000 description 2
- 229910052878 cordierite Inorganic materials 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
- 230000005484 gravity Effects 0.000 description 2
- 238000002347 injection Methods 0.000 description 2
- 239000007924 injection Substances 0.000 description 2
- AMWRITDGCCNYAT-UHFFFAOYSA-L manganese oxide Inorganic materials [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 2
- 230000000873 masking effect Effects 0.000 description 2
- 239000003607 modifier Substances 0.000 description 2
- 239000003921 oil Substances 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 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
- 230000009467 reduction Effects 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 238000000638 solvent extraction Methods 0.000 description 2
- 238000003860 storage Methods 0.000 description 2
- 239000004094 surface-active agent Substances 0.000 description 2
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 2
- 229910052725 zinc Inorganic materials 0.000 description 2
- 239000011701 zinc Substances 0.000 description 2
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 1
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 1
- 229910020197 CePO4 Inorganic materials 0.000 description 1
- 101710178035 Chorismate synthase 2 Proteins 0.000 description 1
- 101710152694 Cysteine synthase 2 Proteins 0.000 description 1
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- 229910002637 Pr6O11 Inorganic materials 0.000 description 1
- CZMRCDWAGMRECN-UGDNZRGBSA-N Sucrose Chemical compound O[C@H]1[C@H](O)[C@@H](CO)O[C@@]1(CO)O[C@@H]1[C@H](O)[C@@H](O)[C@H](O)[C@@H](CO)O1 CZMRCDWAGMRECN-UGDNZRGBSA-N 0.000 description 1
- 229930006000 Sucrose Natural products 0.000 description 1
- 150000001242 acetic acid derivatives Chemical class 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- 150000001412 amines Chemical class 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 239000002981 blocking agent Substances 0.000 description 1
- 230000000903 blocking effect Effects 0.000 description 1
- 229910001593 boehmite Inorganic materials 0.000 description 1
- 229910052796 boron Inorganic materials 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 239000011575 calcium Substances 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000012876 carrier material Substances 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 150000003841 chloride salts Chemical class 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 230000008878 coupling Effects 0.000 description 1
- 238000010168 coupling process Methods 0.000 description 1
- 238000005859 coupling reaction Methods 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 238000007598 dipping method Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 239000002019 doping agent Substances 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000003628 erosive effect Effects 0.000 description 1
- 150000002148 esters Chemical class 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 238000009472 formulation Methods 0.000 description 1
- CJNBYAVZURUTKZ-UHFFFAOYSA-N hafnium(IV) oxide Inorganic materials O=[Hf]=O CJNBYAVZURUTKZ-UHFFFAOYSA-N 0.000 description 1
- 239000002638 heterogeneous catalyst Substances 0.000 description 1
- BHEPBYXIRTUNPN-UHFFFAOYSA-N hydridophosphorus(.) (triplet) Chemical compound [PH] BHEPBYXIRTUNPN-UHFFFAOYSA-N 0.000 description 1
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 1
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 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
- 150000002823 nitrates Chemical class 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- TVMXDCGIABBOFY-UHFFFAOYSA-N octane Chemical compound CCCCCCCC TVMXDCGIABBOFY-UHFFFAOYSA-N 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- 230000003534 oscillatory effect Effects 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 238000002161 passivation Methods 0.000 description 1
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 239000011574 phosphorus Substances 0.000 description 1
- 239000002798 polar solvent Substances 0.000 description 1
- 238000005086 pumping Methods 0.000 description 1
- 238000004904 shortening Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000005720 sucrose Substances 0.000 description 1
- LSNNMFCWUKXFEE-UHFFFAOYSA-L sulfite Chemical class [O-]S([O-])=O LSNNMFCWUKXFEE-UHFFFAOYSA-L 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 238000009827 uniform distribution Methods 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
- OMSYGYSPFZQFFP-UHFFFAOYSA-J zinc pyrophosphate Chemical compound [Zn+2].[Zn+2].[O-]P([O-])(=O)OP([O-])([O-])=O OMSYGYSPFZQFFP-UHFFFAOYSA-J 0.000 description 1
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Abstract
本发明涉及一种催化剂，所述催化剂包括在基材端部a和b之间延伸的长度L的载体基材以及两个洗涂层区A和B，其中洗涂层区A包含第一铂族金属并且从基材端部a开始在该长度L的一部分上延伸，并且洗涂层区B包含与洗涂层区A相同的组分以及另外的第二铂族金属，并且从基材端部b在该长度L的一部分上延伸，其中L＝LA+LB，其中LA是洗涂层区A的长度并且LB是基材长度B的长度。
Description
本发明涉及一种用于处理以主要化学计量的空气/燃料比运行的燃烧式发动机的废气的三元催化剂(TWC)。
在燃烧式发动机领域中众所周知，燃料燃烧是不完全的，并且会产生污染物排放，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)。为了改善空气质量，制定了排放限制法规，以实现来自固定应用以及来自移动源的污染物的较低排放。对于如客车的移动源，已经进行了主动策略诸如改善的燃烧和优化的A/F或λ控制的实施，以努力减少污染物的排放。改善燃料-空气混合(A/F比)作为主要措施大幅减少了污染物。然而，由于这些年以来更为严格的法规，使用非均相催化剂在所难免。
对于汽油发动机，所谓的三元催化剂(TWC)能够消除HC、CO和NOx。此类催化剂包含作为催化活性材料的一种或多种铂族金属，特别是铂、钯和/或铑。
在λ＝1+/-0.005附近，即空气/燃料比等于14.56的情况下，TWC的使用最佳。高于这些值，废气据称是稀薄的并且含有过量的氧化剂，诸如O2和NOx，并且CO和HC被催化氧化成二氧化碳和水。低于该值，废气据称是富集的并且含有过量的还原剂，诸如H2、CO和HC，并且主要使用例如CO作为还原剂将NOx还原为氮气。
在λ＝1时，实现HC、CO和NOx的最佳转化率。然而，汽油发动机是在振荡状况下，即处于略微稀薄和略微富集的条件之间操作。为了拓宽TWC的最佳操作，将铈-锆混合氧化物形式的储氧组分(OSC)包含在其配方中。
高度浓缩的铂族金属(PGM)如铂、钯和铑可在许多废气处理后应用中提供显著的性能改善。因此，就钯而言，从20g/ft3(0.7g/l)的低钯载量到中等至严重老化后的100g/ft3(3.5g/l)的高载量，起燃性能可改善100℃(测量为50％转化率的温度)。性能确实改善成高于这些载量，但是相对于钯载量的性能梯度是低的，并且需要非常高的钯载量以获得显著的影响。预计铑在TWC应用中有相同的一般趋势。
然而，三元转化催化剂中的高浓度铂族金属由于其高成本而并非首选。该缺点可通过将金属策略性放置成例如靠近发动机歧管定位且具有高单元密度的小尺寸单块来部分地克服。这些策略利用了较热的废气温度，缩短了冷启动的时间，因为单块会较快地加热，并且较低的质量外加高单元密度利用了较低的热惯性外加至紧密偶联(CC)单块的较快热传递。
用于改善起燃和用于降低铂族金属成本的另一个策略是将其选择性地定位在单块的一小部分上，通常小于单块体积的10％，在该体积中其具有最大益处。这允许在不使用大量铂族金属的同时浓缩铂族金属，因为铂族金属被策略性地定位在单块的小体积部分上。
在文献中已知的是，当被施加到基材入口时，高度浓缩和短区的铂族金属由于改善的起燃而提供改善的冷启动性能，尤其是对于碳氢化合物(HC)而言，因为当发动机冷却并且燃烧不完全时，高浓度的HC被排出。然而，紧密偶联单块可能在车辆的寿命期间暴露于保持在适当位置的多种污染物。这些包括在发动机油中的被分解或部分燃烧的组分，并且包括钙、磷、锌和硼。这些毒物不是均匀地沉积在单块的长度上，而是优选地朝向催化剂的入口沉积，并且当朝向单块出口行进时，它们的载量会快速下降。载量的下降实际上可为指数级的，使得单块的前一至两英寸可能具有非常高载量的这些组分。根据毒物进入废气的方式，观察到两种不同类型的中毒模式。如果毒物泄漏到车辆燃烧室中，则所得的磷和锌会渗入位于单块上的洗涂层并且与其组分(诸如铈、铝和其他组分)反应。据信，例如，磷在这种中毒机制中会形成磷酸，并且其反应程度使得通常结构稳定的Ce-Zr混合氧化物分解得到新化合物。在极端情况下，铈可从Ce-Zr混合氧化物中提取以得到CePO4，这导致OSC性能损失。在第二机制中，发动机油在其离开燃烧气缸之后可能直接泄漏到废气中。在这种情况下，将油直接沉积到单块洗涂层上并且分解以在表面上产生焦磷酸锌。如果经由该机制沉积高水平，则会在洗涂层表面上形成表面“釉面”或不可渗透屏障，使得废气分子无法扩散到洗涂层内的活性铂族金属组分。这通常被称为掩蔽，并且常见于严重油中毒的TWC催化剂。这种类型中毒的结果是，铂族金属带或区朝向单块的入口面的选择性放置将是反向产生的，因为高分数的昂贵铂族金属无法用于催化剂。预期这种类型的中毒在将来将更为常见，因为行业转向了更为有效的被设计来满足新的
燃料经济性标准的车辆。这作为改善燃料经济性的一个解决方案出现，即使用在更高RPM下操作的更热和更小的发动机。该方法导致更大的发动机磨损，并且预期发动机油的中毒程度会随着这些高燃料经济型车辆的引入而增加。如果入口面受到源自歧管区的颗粒物诸如铁锈的冲击，则选择性地针对单块的入口区的其他中毒机制包括洗涂层侵蚀以及洗涂层的物理阻塞和涂覆。在世界上的一些地区诸如中国，包含辛烷改善剂甲基-环-戊二烯基三羰基锰(MMT)可在入口单块区上分解，以获得Mn3O4层，该Mn3O4层同样可用作必须渗透到洗涂层中以发生催化的废气的物理掩蔽剂或阻断剂。
本发明的发明人讨论了是否可以通过将高铂族金属带或区定位在离单块的入口区足够远或足够靠后的位置来克服将具有高铂族金属浓度的单块的入口区分区或分带的以上缺点，使得以上中毒和钝化机制最小化，同时仍然实现车辆上的改善起燃和随后更短的冷启动周期的优点。虽然将区放置在远离入口区和出口区两者的基材内部体积内可能是不可行的，但是可能获得将第一紧密偶联催化剂的出口分区的优点。在现代应用中，单块尺寸已显著减小，并且单元密度增加。小的高单元密度基材的使用标准现在是600cpsi/2密耳、750cpsi/2密耳和900cpsi/2密耳基材作为第一紧密偶联催化剂(CC-1)的标准。较小体积的基材的另一个原因是靠近车辆歧管位置的空间的限制。
本发明人最终意外观察到，相比于对入口进行分区或在单块的整个体积上使用均匀的铂族金属分布，对CC-1单块的出口进行分区会导致可测量的性能优势。本说明的部分可源自如上文所述的入口的选择性中毒外加当前CC-1单块的特殊特性(较小体积、较短部件、较低质量和较高单元密度)。
因此，本发明涉及一种催化剂，所述催化剂包括在基材端部a和b之间延伸的长度L的载体基材以及两个洗涂层区A和B，其中
洗涂层区A包含第一铂族金属并且从基材端部a开始在所述长度L的一部分上延伸，并且
洗涂层区B包含与洗涂层区A相同的组分以及另外的第二铂族金属并且从基材端部b在所述长度L的一部分上延伸，
其中L＝LA+LB，其中LA是洗涂层区A的长度并且LB是基材长度B的长度。
因此，根据本发明，第一铂族金属均匀地分布在载体基材的整个长度L上，而第二铂族金属仅存在于洗涂层区B中。
因此，洗涂层区B中铂族金属的总量高于洗涂层区A中铂族金属的总量。
第一铂族金属和第二铂族金属可以是相同的或可以是不同的。例如，第一铂族金属为铂、钯和/或铑，并且第二铂族金属为钯或铑。优选地，第一铂族金属为钯和铑，并且第二铂族金属为钯，或者第一铂族金属为钯和铑，并且第二铂族金属为铑。
在第一铂族金属和第二铂族金属均相同(例如钯)的情况下，洗涂层区B包含比洗涂层区A更高量的铂族金属(例如钯)。
在本发明的实施方案中，洗涂层区A包括两个层A1和A2，该两个层A1和A2均在该长度LA上延伸，其中层A1包含第一铂族金属，并且层A2包含不同于层A1的该第一铂族金属的第一铂族金属，并且洗涂层区B包括两个层B1和B2，该层B1和B2均在长度LB上延伸，其中层B1包含与层A1相同的组分，并且层B2包含与层A2相同的组分，并且其中层B1和B2包含另外的第二铂族金属。
在本发明的实施方案中，层A1包含钯或包含钯和一种或多种另外的铂族金属，特别是铂和铑，优选铑。
优选地，层A1中的第一铂族金属为钯，并且层A2中的第一铂族金属为铑。在这种情况下，重量比Pd:Rh为例如10:1至10:1。
在本发明的实施方案中，层A2包含铑或包含铑和一种或多种另外的铂族金属，特别是铂和钯，优选钯。在后一种情况下，重量比Pd:Rh为例如10:1至1:10。
在本发明的优选实施方案中，除了洗涂层区B中存在第二铂族金属之外，洗涂层区A和B是相同的。
同样，除了层B1中存在第二铂族金属之外，层A1和B1是相同的，并且除了层B2中存在第二铂族金属之外，层A2和B2是相同的。
优选地，第一铂族金属和第二铂族金属彼此独立地承载在载体材料上。
作为载体材料，可以使用本领域技术人员已知的所有材料用于该目的。通常，它们的BET表面积为30m2/g至250m2/g，优选100m2/g至200m2/g(根据德国标准DIN 66132确定)，并且特别是选自由以下项组成的组：氧化铝、二氧化硅、氧化镁、二氧化钛、氧化锆、二氧化铈、包含这些材料中的至少两种的混合物以及包含这些材料中的至少两种的混合氧化物。
优选氧化铝、氧化铝/二氧化硅混合氧化物、氧化镁/氧化铝混合氧化物、二氧化铈、二氧化铈/氧化锆混合氧化物和沸石。
在使用氧化铝的情况下，优选例如用1重量％至6重量％、特别是4重量％的氧化镧使其稳定。
不同的铂族金属可承载在相同或不同的载体材料上。
在洗涂层区A和A1中的铂族金属分别包含钯的情况下，基于载体基材的区体积并以钯金属计算，其通常以0.04g/l至4.0g/l的量存在。洗涂层区B中的钯含量高于洗涂层区A中的钯含量，并且基于载体基材的体积并以钯金属计算，其通常为2g/l至20g/l。
在洗涂层区A和A1中的铂族金属分别包含铑的情况下，基于载体基材的区体积并且并以铑金属计算，其通常以0.04g/l至4.0g/l的量存在。
在本发明的实施方案中，洗涂层区A在载体基材的长度L的70％至95％、优选73％至90％上延伸，并且洗涂层区B在载体基材的长度L的5％至30％、优选10％至27％上延伸。
在本发明的实施方案中，长度L的载体基材可为流通式基材或过滤基材。通常由堇青石或金属制成的这种载体基材在文献中有述，并且可在市场上购买。
本发明的催化剂可由已知方法制造特别是由两步法制造，该方法包括：
·用涂层悬浮液(洗涂层)涂覆所述载体基材，所述涂层悬浮液在所述载体基材的整个长度L上含有洗涂层区A的组分，以及
·将涂覆的载体基材浸渍在含有所述第二铂族金属的水溶性化合物的水溶液中，直到与洗涂层区B的该长度对应的长度，以便形成洗涂层区B。
第一步骤中的涂覆通常经由常规的浸渍、抽吸和泵送方法进行，这些方法在文献中被广泛描述并且是本领域的技术人员已知的。
用于第二步骤中的第二铂族金属的水溶性化合物可为任何稳定的铂族金属盐，包括硝酸盐、乙酸盐、氯化物、亚硫酸盐、胺络合物等。由于溶剂(诸如水)的芯吸在与铂族金属溶液接触之后发生，因此通常需要添加表面活性剂或表面张力调节剂以控制该现象，因为在没有该表面活性剂或表面张力调节剂的情况下无法控制带长度。避免芯吸和不受控制的带长度也可通过使用除水之外的溶剂诸如醇(甲醇或乙醇)、其他极性溶剂诸如四氢呋喃(THF)、酯等来实现。事实上，可使用铂族金属盐可溶于其中的任何溶剂。铂族金属吸收基于带的长度、溶液吸收的体积和溶液的铂族金属浓度来控制。施加带的优选方法是计量电荷方法，其中注入的所有溶液在整个部件处置、干燥和煅烧过程中保留在该部件上。期望溶液不与单块上的洗涂层区A相互化学作用，使得洗涂层组分被溶解和提取。由于高浓度带的施加是在施加洗涂层区A之后完成的，因此该方法非常灵活，并且在洗涂层组合物或洗涂层通过次数方面不是技术专有的。
第一步骤和第二步骤之后通常是煅烧和任选地在含有形成气体的气氛中进行热还原。
本发明的催化剂适用于处理以主要化学计量的空气/燃料比运行的发动机的废气，该废气的处理通过使废气经过本发明的催化剂来进行。具体地讲，本发明的催化剂可以有利地用于紧密偶联的位置，优选地用作直接位于排气歧管后面(所谓的CC-1位置)的第一催化剂。
因此，本发明还涉及一种用于处理以主要化学计量的空气/燃料比运行的发动机的废气的方法，其特征在于，该废气经过本发明的催化剂，其中该废气在基材端部a处进入该催化剂并且在基材端部b处离开催化剂。
在该方法的一个优选实施方案中，本发明的催化剂被布置在紧密偶联的位置，特别是直接布置在排气歧管后面。
本发明的催化剂可合并另一三元催化剂以形成三元催化剂体系。
例如，本发明的催化剂的基材端部b之后可以是常规的三元催化剂。
另外，本发明的催化剂的基材端部b可跟随常规的三元催化剂。
作为常规的三元催化剂，可使用本领域技术人员已知的且文献中所述的所有三元催化剂。通常，它们包含承载在载体材料上的铂族金属，特别是钯和铑，以及特别是铈-锆混合氧化物的储氧组分(OSC)。
图1示出了根据本发明的催化剂。附图的上部示出了本发明催化剂(1)的细节，该催化剂包括载体基材(3)，该载体基材在基材端部a和b之间延伸并且承载洗涂层区A(4)和洗涂层区B(5)。
附图的下部示出了本发明的另一个实施方案的细节。催化剂(2)包括载体基材(3)，该载体基材在基材端部a和b之间延伸。洗涂层区A包括层A1(6)和A2(7)，而洗涂层区B包括层B1(9)和层B2(8)。层A1(6)和B1(9)的不同之处仅在于B1(9)包含与A1(6)相比的第二铂族金属。同样，层A2(7)和B2(8)的不同之处仅在于B2(8)包含与A2(7)相比的第二铂族金属。
图2示出了根据本发明的催化剂体系。
上部示出了本发明的催化剂体系(11)，该催化剂体系包含本发明的催化剂(1)和常规的三元催化剂(10)。两种催化剂被布置成使得洗涂层区B(5)之后是常规的三元催化剂(10)。
下部示出了本发明的催化剂体系(12)，该催化剂体系包含本发明的催化剂(1)和常规的三元催化剂(10)。两种催化剂均被布置成使得洗涂层区B(5)跟随常规的三元催化剂(10)。
比较例1
比较例1是2层Pd/Rh技术，其制备如下：
a)对于第1层(Pd层)，通过首先将硝酸以1重量％加入水中来制备浆液。然后在搅拌下加入BaSO4，之后添加OSC物质。OSC物质由CeO2＝44重量％、ZrO2+HfO2＝42重量％、La2O3＝9.5重量％和Pr6O11＝4.5重量％组成。将浆液搅拌15分钟，并且然后缓慢添加氧化铝。搅拌30分钟后，添加基于固体计10重量％的蔗糖，并且最后添加可分散的勃姆石粘结剂。然后使用Sweco型研磨机将浆液研磨至大于2微米的平均粒度，90％的直径分布为6.0至7.0微米，并且100％通过小于25微米(即，100％的颗粒具有小于25微米的粒度)。然后称量浆液，并且在540℃下测量LOI(烧失量)以确定总煅烧固体含量。基于该值计算Pd载量。然后在搅拌的同时，将硝酸钯溶液滴加到浆液中。在Pd添加后，浆液比重在1.49至1.52的范围内。
B)通过将蜂窝陶瓷单块(由堇青石制成的可商购获得的流通式基材(3.54”×5.16”×2.5”长；900cpsi/2密耳)浸渍在洗涂层浆液中，之后使用真空将浆液向上抽吸到通道中，执行涂覆。然后从浆液中移除单块，并且通过向其另一端部施加真空来清除通道。通过改变比重和其他涂层参数(诸如真空时间和抽吸到蜂窝通道中的浆液的量)来控制洗涂层载量。在施加洗涂层之后，将单块在540℃下煅烧2小时。基于干燥煅烧，最终WC载量为氧化铝溶胶＝3g/L，稳定的氧化铝＝52g/L，BaSO4＝15g/L且OSC＝34g/L，得到层1的总载量＝104g/L。在单块的总长度上涂覆该层。
c)然后对第二层(Rh层)重复该过程，不同的是添加Rh而不是Pd。基于干燥煅烧，最终WC载量为氧化铝溶胶＝3g/L，稳定的氧化铝＝34g/L，BaSO4＝6g/L且OSC＝49g/L，得到层2的总载量＝92g/L。在单块的总长度上也涂覆第二层。
将所得产物干燥并且煅烧。所获得的催化剂随后称为CC1。
实施例1
将根据比较例1获得的CC1浸渍在硝酸钯水溶液中以便形成1.25”长度的区，该区包含总共246g/ft3(8,69g/l)的钯。将所得产物干燥并且煅烧。所获得的催化剂随后称为C1。
CC1和C1的比较
a)使用4模式老化循环将CC1和C1引擎老化至有效(全部使用寿命)150K英里条件，持续90小时。每个4模式循环持续60秒，并且将老化循环重复4500次。使用添加剂DMA4作为掺杂剂，用磷掺杂的燃料完成前50小时的老化。剩余的40小时仅为热老化。各个模式为：化学计量、富燃、富燃+空气注入和化学计量+空气注入。在CC1和C1催化剂中测得的峰值温度为约990℃。老化的详细描述在2016年SAE世界会议论文2016-01-0925中给出。
b)使用Ford Escape 2.0L GTDI(4XFTP/US06)在车辆测试中测试老化催化剂C1。催化剂被布置直接在排气歧管后面的紧密偶联的位置。废气在基材端部a上进入催化剂，并且使其留在钯量增加246g/ft3(8,69g/l)(基材端部b)的侧上。该测试的结果在图3中作为“测试C1 a”给出。
c)重复b)中所述的测试，不同的是废气在钯量增加246g/ft3(8,69g/l)的侧(基材端部b)上进入催化剂并且留在其上(基材端部a)。该测试的结果在图3中作为“测试C1 b”给出。
d)重复b)中所述的测试，不同的是使用催化剂CC1。该测试的结果在图3中作为“测试CC1”给出。
e)图3分别示出了测试C1 a、C1 b和CC1中获得的THC排放(以mg/英里为单位称量)。
比较例2
重复比较例1，不同的是在基材的总长度上涂覆96g/ft3(3.4g/l)的钯和4g/ft3(0.14g/l)的铑。
将获得的基材中的两个合并以形成随后被称为CCS1的催化剂体系。
实施例2
将催化剂CC1与催化剂C1合并以形成催化剂体系。催化剂被布置成使得废气首先进入催化剂C1的基材端部a，并且在基材端部b处离开催化剂C1之后进入催化剂CC1。由此获得的催化剂体系随后称为CS1。
实施例3
将催化剂CC1与催化剂C1合并以形成催化剂体系。催化剂被布置成使得废气首先进入催化剂C1并且在离开之后，在基材端部b处进入催化剂C1。由此获得的催化剂体系随后被称为CS2。
CCS1、CS1和CS2的比较
根据以上步骤a)和b)老化并且测试CCS1、CS1和CS2。图4示出了由此获得的THC排放(以mg/英里为单位称量)。
Claims (17)
1.催化剂，所述催化剂包括在基材端部a和b之间延伸的长度L的载体基材以及两个洗涂层区A和B，其中
洗涂层区A包含第一铂族金属并且从基材端部a开始在所述长度L的一部分上延伸，并且
洗涂层区B包含与洗涂层区A相同的组分以及另外的第二铂族金属并且从基材端部b在所述长度L的一部分上延伸，
其中L＝LA+LB，其中LA是洗涂层区A的长度并且LB是基材长度B的长度。
2.根据权利要求1所述的催化剂，其中第一铂族金属和第二铂族金属是相同的或不同的。
3.根据权利要求1和/或2所述的催化剂，其中所述第一铂族金属为铂、钯和/或铑，并且所述第二铂族金属为钯或铑。
4.根据权利要求1至3中的一项或多项所述的催化剂，其中所述第一铂族金属为钯和铑，并且所述第二铂族金属为钯。
5.根据权利要求1至4中的一项或多项所述的催化剂，其中洗涂层区A包括两个层A1和A2，所述两个层A1和A2均在所述长度LA上延伸，其中层A1包含第一铂族金属，并且层A2包含不同于层A1的所述第一铂族金属的第一铂族金属，并且洗涂层区B包括两个层B1和B2，所述层B1和B2均在所述长度LB上延伸，其中层B1包含与层A1相同的组分，并且层B2包含与层A2相同的组分，并且其中层B1和B2包含另外的第二铂族金属。
6.根据权利要求5所述的催化剂，其中层A1中的所述第一铂族金属为钯和/或铑，并且层A2中的所述第一铂族金属为铑。
7.根据权利要求5所述的催化剂，其中层A1中的所述第一铂族金属为钯和铑，并且重量比Pd:Rh为10:1至1:10。
8.根据权利要求1至7中的一项或多项所述的催化剂，其中所述第一铂族金属和所述第二铂族金属彼此独立地承载在载体材料上。
9.根据权利要求8所述的催化剂，其中所述载体材料选自由以下项组成的组：氧化铝、二氧化硅、氧化镁、二氧化钛、氧化锆、二氧化铈、包含这些材料中的至少两种的混合物以及包含这些材料中的至少两种的混合氧化物。
10.根据权利要求1至9中的一项或多项所述的催化剂，其中洗涂层区A在所述载体基材的所述长度L的70％至95％上延伸，并且洗涂层区B在所述载体基材的所述长度L的5％至30％上延伸。
11.根据权利要求1至10中的一项或多项所述的催化剂，其中所述长度L的所述载体基材是流通式基材或过滤基材。
12.用于通过两步法制造根据权利要求1至11中的一项或多项所述的催化剂的方法，所述方法包括：
·用涂层悬浮液(洗涂层)涂覆所述载体基材，所述涂层悬浮液在所述载体基材的整个长度L上含有洗涂层区A的组分，以及
·将涂覆的载体基材浸渍在含有所述第二铂族金属的水溶性化合物的水溶液中，直到与载体涂层区B的长度对应的长度，以便形成洗涂层区B。
13.催化剂体系，所述催化剂体系包含根据权利要求1至11中的一项或多项所述的催化剂和另一种三元催化剂。
14.根据权利要求13所述的催化剂体系，其中根据权利要求1至11中的一项或多项所述的催化剂的基材端部b之后是常规的三元催化剂。
15.根据权利要求13所述的催化剂体系，其中根据权利要求1至11中的一项或多项所述的催化剂的基材端部b跟随常规的三元催化剂。
16.处理燃烧式发动机的废气的方法，其中所述废气经过权利要求1至11中的一项或多项所述的催化剂，其中所述废气在基材端部a处进入所述催化剂并且在基材端部b处离开所述催化剂。
17.根据权利要求16所述的方法，其中权利要求1至11中的一项或多项所述的催化剂被布置在紧密偶联的位置中。
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| EP3793723A1 (en) | 2021-03-24 |
| CN112135685B (zh) | 2023-09-01 |
| WO2019219812A1 (en) | 2019-11-21 |
| US11161098B2 (en) | 2021-11-02 |
| US20190351394A1 (en) | 2019-11-21 |
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