CN106795445A - 减少实际行驶循环颗粒物排放量的燃料组合物以及配制该燃料组合物的方法 - Google Patents
减少实际行驶循环颗粒物排放量的燃料组合物以及配制该燃料组合物的方法 Download PDFInfo
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- CN106795445A CN106795445A CN201580055375.0A CN201580055375A CN106795445A CN 106795445 A CN106795445 A CN 106795445A CN 201580055375 A CN201580055375 A CN 201580055375A CN 106795445 A CN106795445 A CN 106795445A
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- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 150000002460 imidazoles Chemical class 0.000 description 1
- WRSXUNSJGJUKHE-UHFFFAOYSA-N indazole Chemical compound C1=CC=C[C]2C=NN=C21 WRSXUNSJGJUKHE-UHFFFAOYSA-N 0.000 description 1
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- 239000011159 matrix material Substances 0.000 description 1
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- NFWSQSCIDYBUOU-UHFFFAOYSA-N methylcyclopentadiene Chemical compound CC1=CC=CC1 NFWSQSCIDYBUOU-UHFFFAOYSA-N 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 125000000740 n-pentyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 1
- YHVAHDISAMDYQA-UHFFFAOYSA-N nitric acid;octane Chemical compound O[N+]([O-])=O.CCCCCCCC YHVAHDISAMDYQA-UHFFFAOYSA-N 0.000 description 1
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- 125000002347 octyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
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- 230000008520 organization Effects 0.000 description 1
- SLIUAWYAILUBJU-UHFFFAOYSA-N pentacene Chemical compound C1=CC=CC2=CC3=CC4=CC5=CC=CC=C5C=C4C=C3C=C21 SLIUAWYAILUBJU-UHFFFAOYSA-N 0.000 description 1
- RGSFGYAAUTVSQA-UHFFFAOYSA-N pentamethylene Natural products C1CCCC1 RGSFGYAAUTVSQA-UHFFFAOYSA-N 0.000 description 1
- 229920005547 polycyclic aromatic hydrocarbon Polymers 0.000 description 1
- 125000005575 polycyclic aromatic hydrocarbon group Chemical group 0.000 description 1
- 230000008092 positive effect Effects 0.000 description 1
- 125000001436 propyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 150000003217 pyrazoles Chemical class 0.000 description 1
- PBMFSQRYOILNGV-UHFFFAOYSA-N pyridazine Chemical compound C1=CC=NN=C1 PBMFSQRYOILNGV-UHFFFAOYSA-N 0.000 description 1
- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 description 1
- 150000003233 pyrroles Chemical class 0.000 description 1
- JWVCLYRUEFBMGU-UHFFFAOYSA-N quinazoline Chemical compound N1=CN=CC2=CC=CC=C21 JWVCLYRUEFBMGU-UHFFFAOYSA-N 0.000 description 1
- 238000007670 refining Methods 0.000 description 1
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- 150000005846 sugar alcohols Polymers 0.000 description 1
- HVZJRWJGKQPSFL-UHFFFAOYSA-N tert-Amyl methyl ether Chemical compound CCC(C)(C)OC HVZJRWJGKQPSFL-UHFFFAOYSA-N 0.000 description 1
- AZAKMLHUDVIDFN-UHFFFAOYSA-N tert-butyl nitrate Chemical compound CC(C)(C)O[N+]([O-])=O AZAKMLHUDVIDFN-UHFFFAOYSA-N 0.000 description 1
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Classifications
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- C—CHEMISTRY; METALLURGY
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Abstract
为了共混燃料以满足具体的法规和行业要求例如辛烷值要求，可以使用具有不同辛烷值的共混组分。一种添加的组分包括具有较高芳烃含量的组合物。遗憾的是，当高芳烃燃料在内燃机中燃烧时，这种芳烃含量可能增加内燃机的颗粒物排放量。如本申请解释，减少芳烃含量和用可替代的辛烷值助剂代替该辛烷值提高要求得到了下述配制的燃料，该燃料在实际行驶该内燃机时具有较低的颗粒物排放量，与具有较高芳烃含量的燃料相比。
Description
相关申请的交叉引用
本申请享有2014年10月17日提交的题为“FUEL COMPOSITION AND METHOD OFFORMULATING A FUEL COMPOSITION TO REDUCE REAL-WORLD DRIVING CYCLE PARTICULATEEMISSIONS”的美国专利申请序列号14/516,627的优先权，其内容完全通过参考并入本申请。
技术领域
本发明的技术领域是内燃机燃料和配制方法。具体地，本发明涉及与具有相对较高芳烃含量的可比燃料相比当燃烧时产生较少颗粒物排放量的燃料。
背景技术
车辆排放标准通常在全球越来越受到环境监管组织的严密检查。标准的设置越来越要求越来越低量的各种类型排放物。特别是，车辆颗粒物排放限值正在显著降低。这包括来自汽油/火花点燃发动机以及其它发动机技术的颗粒物排放量的限值。
在火花点燃发动机中，颗粒物排放量的降低限值一部分靠改善车辆硬件设计来解决。正在考虑喷油技术来改善燃烧。如果不予优化，例如，喷油器结焦可能得到不利的燃料喷雾以及增加颗粒物排放量。因此，正在发展技术以改善硬件性能，由此减少颗粒物排放量。
在传统行驶循环测试中测量排放物例如颗粒物排放物；但是，这些传统测试不足以再现实际行驶条件。因此，传统测试结果可能无法代表在实际行驶过程中的车辆排放情况。
发明内容
因此，本发明的目的是通过改善燃料组合物减少实际行驶循环颗粒物排放量。已经发现，燃料芳烃含量与颗粒物排放量密切相关。也就是说，相对较高的燃料芳烃含量导致相对较高的颗粒物排放量。通过减少芳烃含量和用具有减少的芳烃含量或无芳烃含量的辛烷值助剂例如有机金属辛烷值助剂代替该芳烃含量，积极的成效是在不损害辛烷值和燃料效率的情况下减少颗粒物排放量。
在一个实例中，减少内燃机颗粒物排放量的方法首先是提供芳烃含量为至少约10体积％的基础燃料。接着，所述方法包括向该基础燃料中添加一定量的辛烷值助剂以形成燃料制剂，其中辛烷值助剂与基础燃料的混合物的芳烃含量少于在不存在所述辛烷值助剂的情况下基础燃料的芳烃含量。与来自基础燃料燃烧的颗粒物排放量相比，来自所述燃料制剂燃烧的颗粒物排放量减少了，通过总颗粒数(total particle number)(PN)测得。
附图说明
图1是图表，说明三种可比燃料制剂—基础燃料、包含辛烷值助剂的燃料、和重整燃料的研究法辛烷值(RON)、马达法辛烷值(MON)、和芳烃含量。
图2是图表，说明图1所示的三种燃料的蒸馏曲线。
图3是图表，显示在常见ARTEMIS行驶循环(Common ARTEMIS Driving Cycles)(CADC)的子循环—市区、郊外和M150期间的颗粒物排放数(PN)(固体和挥发物两者)。
图4是图表，说明在高速-高负载操作条件下的颗粒物和一氧化碳(CO)瞬时排放率。
图5是图表，说明在高速-高负载操作条件下的瞬时颗粒物排放率和空燃比(AFR)。
具体实施方式
为了共混燃料以满足具体的辛烷值要求，可以使用具有不同辛烷值的共混组分。成品燃料中的详细组分最终确定燃料的物理化学性质，因此确定产生于燃料燃烧的车辆废气排放量。本申请公开的方法通过使用辛烷值助剂例如包含甲基环戊二烯三羰基锰的那些来减少实际行驶循环颗粒物排放量，由此燃料可以在减少燃料共混物中芳烃含量的同时又可满足辛烷值要求。
新的和正在发展的燃料组合物要求可能在很多情况下导致成品燃料具有高芳烃含量。必须添加芳烃，以使燃料具有给定规范内要求的必要辛烷值。这些高度精炼的燃料可以包括至少10％的芳烃含量、或可替换地为至少25％的芳烃含量、或再进一步可替换地为至少35％的芳烃含量。这种相对高的芳烃含量确保满足辛烷值要求。但是，已经确定这种芳烃含量是大量颗粒物排放的来源。
现代精炼要求也包括在所得燃料中硫的量不断下降。这些燃料可以包含少于50ppm的硫、或可替换地为少于15ppm的硫、或再进一步可替换地为少于10ppm的硫。为了在各种氢化工艺中进行这种燃料脱硫，一个结果是所得精炼燃料的辛烷值损失。这种辛烷值损失必须通过添加其它具有相对较高辛烷值的共混组分来补偿。那些组分包括早先确定的高芳烃含量组分。
现有精炼法的另一个副作用是所得燃料馏分的蒸馏曲线具有物理变化。公知的蒸馏燃料馏分称为T10，T50，和T90。T90馏分通常反映燃料中相对重质化合物的挥发性。T90数越高，燃料的该馏分越难蒸发。认为这会降低完全燃烧的容易度，导致形成较高的颗粒物排放量和沉积物。对于本申请所述的燃料馏分和基础燃料，T90为至少约140℃。该T90相对高于目前尚未精炼的燃料的典型历史T90数。
在高速-高负载操作条件下，例如在常见ARTEMIS行驶循环(CADC)的高速公路150上猛踩油门加速，由于燃料增浓以适应所需动力和/或催化剂保护，可能发生不完全燃烧。与在传统管理循环(例如新欧洲行驶循环(NEDC))中使用相比，这种类型的行驶特征在实际使用中更常观察到，且排放物贡献较高，更能代表实际排放清单。车辆颗粒物排放量可极大地受燃料组成以及它们被氧化的容易性的影响。那些极高颗粒物排放突出通过在那些特定的操作模式下同时发生的CO排放突出来确定。将燃料与有机金属辛烷值助剂共混、而不是增加芳烃或烯烃含量，可以显著减少颗粒物排放量。
本申请的“燃料”表示适用于燃烧系统操作的一种或多种燃料，包括汽油，汽车和航空的无铅汽油，和所谓的重整汽油，所述重整汽油通常包含汽油沸程范围内的烃和可溶于燃料的氧化的掺和剂两者，所述可溶于燃料的氧化的掺和剂例如为醇、醚和其它适宜的含氧有机化合物。适宜使用的增氧剂(oxygenate)包括甲醇，乙醇，异丙醇，叔丁醇，混合的C1-C5醇，甲基叔丁基醚，叔戊基甲基醚，乙基叔丁基醚，以及混合醚。当使用时，增氧剂在基础燃料中的存在量可以为至多约90体积％，优选为仅至多约25体积％。
如本申请讨论，辛烷值助剂一般包括有机金属辛烷值助剂和其它辛烷值助剂两者。这些其它辛烷值助剂包括醚和芳族胺。
针对用于本申请的目的，重要的是辛烷值助剂和与辛烷值助剂共混的任何载液包含减少的芳烃含量或不包含芳烃含量。重要的是，这些辛烷值助剂必须包含少于20％的芳烃含量，或可替换地为少于10％的芳烃含量，或再进一步可替换地为少于5％的芳烃含量。
一类有机金属辛烷值助剂可以包含锰。含锰有机金属化合物的实例是三羰基锰化合物。
可使用的适宜三羰基锰化合物包括环戊二烯三羰基锰，甲基环戊二烯三羰基锰，二甲基环戊二烯三羰基锰，三甲基环戊二烯三羰基锰，四甲基环戊二烯三羰基锰，五甲基环戊二烯三羰基锰，乙基环戊二烯三羰基锰，二乙基环戊二烯三羰基锰，丙基环戊二烯三羰基锰，异丙基环戊二烯三羰基锰，叔丁基环戊二烯三羰基锰，辛基环戊二烯三羰基锰，十二烷基环戊二烯三羰基锰，乙基甲基环戊二烯三羰基锰，茚基三羰基锰等，包括两种或更多种这些化合物的混合物。一个实例是在室温为液体的环戊二烯三羰基锰，例如甲基环戊二烯三羰基锰、乙基环戊二烯三羰基锰、环戊二烯三羰基锰与甲基环戊二烯三羰基锰的液体混合物、甲基环戊二烯三羰基锰与乙基环戊二烯三羰基锰的混合物等。
含锰化合物在燃料中的量或浓度可以根据很多因素(包括特定燃料的具体特性)来选择。含锰化合物的处理率可以超过100mg锰/升，为至多约50mg锰/升，为约1至约30mg锰/升，或再进一步为约5至约20mg锰/升。
另一类有机金属辛烷值助剂的实例是含铁的那类。这些含铁化合物包括二茂铁。这些含铁化合物的处理率类似于以上含锰化合物的处理率。
硝酸酯辛烷值助剂(也常称为点火改进剂)包括取代或未取代的脂族或脂环族醇的硝酸酯，所述醇可以是一元醇或多元醇。有机硝酸酯可以是取代或未取代的具有至多约10个碳原子(例如，2至10个碳原子)的硝酸烷基酯或硝酸环烷基酯。烷基可以是线形或支化的(或线形烷基和支化烷基的混合物)。适宜用作硝酸酯燃烧改进剂的硝酸酯化合物的具体实例包括但不限于以下化合物：硝酸甲酯，硝酸乙酯，硝酸正丙酯，硝酸异丙酯，硝酸烯丙基酯，硝酸正丁酯，硝酸异丁酯，硝酸仲丁酯，硝酸叔丁酯，硝酸正戊酯，硝酸异戊酯，硝酸2-戊基酯，硝酸3-戊基酯，硝酸叔戊酯，硝酸正己酯，硝酸正庚酯，硝酸仲庚酯，硝酸正辛酯，硝酸2-乙基己酯，硝酸仲辛酯，硝酸正壬酯，硝酸正癸酯，硝酸环戊基酯，硝酸环己基酯，硝酸甲基环己基酯，硝酸异丙基环己基酯等。也适用的是烷氧基取代的脂族醇的硝酸酯，例如硝酸2-乙氧基乙基酯，硝酸2-(2-乙氧基乙氧基)乙基酯，1-甲氧基丙基-2-硝酸酯，和硝酸4-乙氧基丁基酯，以及硝酸二醇酯例如二硝酸1,6-六亚甲基酯等。例如，也包括具有5-10个碳原子的硝酸烷基酯和二硝酸烷基酯，最特别是硝酸伯戊基酯的混合物，硝酸伯己基酯的混合物，和硝酸辛基酯例如硝酸2-乙基己基酯。
实施例
以下给出实施例，其中对三种燃料进行共混和测试。燃料#1是基础燃料。非基础燃料共混物包含80％的基础燃料和20％的HSR、重整燃料或烷基化物的组合，最终的共混燃料如表1中所示标记。三种燃料都具有相等的研究法辛烷值(RON)和马达法辛烷值(MON)，但是芳烃含量却各不相同(图1)。燃料#3具有最高的芳烃含量(41.91体积％)，然后是基础燃料(32.83体积％)，最低的是燃料#2(28.39体积％)，即含MMT的燃料。图2中的蒸馏曲线表明燃料#2相对于其它两种燃料具有显著较高的T50和T90。
表1：燃料共混基质
图3显示常见ARTEMIS行驶循环的颗粒物排放量(固体和挥发物两者的总颗粒数，PN)。很明显，在第3阶段(高速公路部分)，颗粒物排放量远远高于其它两个阶段，约比其它两个阶段高两个数量级。在第3阶段中，燃料#2(与MMT共混的燃料)排放最低的总颗粒物排放量，比基础燃料低23％，比重整燃料低10％。应该注意的是，本申请报告的颗粒物排放量为总颗粒的形式，表示在测量中不仅计算固体也计算挥发物。这是因为，在CADC行驶条件下挥发物可能会变成总颗粒物排放率中的优势成分。在这种条件下除去挥发物可对排放量测量和界定带来显著偏差。
图4中的CO排放峰值和图5中的AFR比迁移一致地显示在该高速-高负载条件下的车辆操作可迫使发动机加浓。在该条件下极高的颗粒物排放量是发动机加浓和不完全燃烧的联合效果。这种非常敏感的体系对于车辆颗粒物排放控制是非常关键的，因为相比于其它操作条件它们的贡献是非常显著的。
本申请使用的术语"辛烷值"是指异辛烷在异辛烷(2,2,4-三甲基戊烷，辛烷的异构体)和正庚烷的混合物中的体积百分比，该混合物与待研究的燃料具有相同的抗爆震(即，抗自然性或抗爆性)能力。
本申请使用的术语研究法辛烷值(RON)是指在苛刻性低的发动机操作下的模拟的燃料性能。本申请使用的术语马达法辛烷值(MON)是指较苛刻的(相比于RON)发动机操作下的模拟的燃料性能，这种操作可能会在高速或高负载下出现。
两种值都使用标准化单缸可变压缩比发动机测量。对于RON和MON两者，发动机以恒定速度(RPM's)操作，且增加压缩比，直到开始爆震。对于RON，发动机速度设定在600rpm，对于MON，发动机速度设定在900rpm。同样，对于MON，将燃料预加热，可变点火正时用于进一步加压燃料的抗爆震性能。
本申请使用的术语“芳烃”用于描述具有带离域电子的共轭平面环系的有机分子。本申请使用的"芳环"可以描述单环，多环，或杂环。此外，"芳环"可以描述为连接但非稠合的芳环。单环也可以描述为芳烃或芳族烃。单环的实例包括但不限于苯，环戊烯，和环戊二烯。多环也可以描述为多芳族烃，多环芳族烃，或多核芳族烃。多环包括稠合芳环，其中单环共用连接键。多环的实例包括但不限于萘，蒽，并四苯，或并五苯。杂环也可以描述为杂芳烃。杂环包含非碳环内原子，其中芳环的至少一个碳原子由杂原子替代，所述杂原子例如但不限于氧、氮、或硫。杂环的实例包括但不限于，呋喃，吡啶，苯并呋喃，异苯并呋喃，吡咯，吲哚，异吲哚，噻吩，苯并噻吩，苯并[c]噻吩，咪唑，苯并咪唑，嘌呤，吡唑，吲唑，唑，苯并唑，异唑，苯并异唑，噻唑，苯并噻唑，喹啉，异喹啉，吡嗪，喹喔啉，吖啶，嘧啶，喹唑啉，哒嗪，或噌啉。
考虑到本申请披露的说明书和实践，本申请的其他实施方式对于本领域技术人员来说将是明显的。如整个说明书和权利要求中使用的，“一个”和/或“一种”可以是指一个或多于一个、一种或多于一种。除非另外指明，否则在说明书和权利要求中使用的表示成分的量，性质例如分子量、百分比、比率和反应条件等的所有数字要理解为在所有情况下均由术语“约”修饰。因此，除非相反指明，否则说明书和权利要求中所述的数值参数均为近似值，其可以根据寻求通过本申请要得到的所需性质变化。至少基于并非试图限制本申请中的等同于权利要求范围的原则，各个数值参数应该至少根据报告的有效数字的数值和通过适用普通舍入技术来解释。尽管本申请宽范围内述及的数值范围和参数均为近似值，但具体实施例中述及的数值均尽可能报告得精确。但是，任何数值本身含有由于它们各自测试测量中所得标准偏差必然引起的某些误差。意在认为说明书和实施例仅为示例性的，本申请的实际范围和精神由所附权利要求来表明。
Claims (14)
1.减少内燃机的颗粒物排放量的方法，所述方法包括以下步骤：
提供基础燃料，所述基础燃料的芳烃含量为至少约10体积％；
向所述基础燃料中添加一定量的辛烷值助剂以形成燃料制剂，其中包含辛烷值助剂和基础燃料的燃料制剂的芳烃含量少于在不存在所述辛烷值助剂的情况下基础燃料的芳烃含量；
其中(1)与来自所述基础燃料燃烧的颗粒物排放量相比，来自所述燃料制剂燃烧的颗粒物排放量减少了，通过颗粒数(PN)(固体和挥发物两者)测得，并且其中(2)与在不存在所述辛烷值助剂的情况下所述基础燃料的辛烷值相比，所述燃料制剂的辛烷值基本相同或较高。
2.如权利要求1所述的减少颗粒物排放量的方法，其中所述基础燃料的芳烃含量为至少约20体积％。
3.如权利要求1所述的减少颗粒物排放量的方法，其中所述基础燃料的芳烃含量为至少约35体积％。
4.如权利要求1所述的减少颗粒物排放量的方法，其中所述燃料制剂还具有至少约5体积％的烯烃含量。
5.如权利要求4所述的减少颗粒物排放量的方法，其中所述燃料制剂的烯烃含量为至少约10％。
6.如权利要求1所述的减少颗粒物排放量的方法，其中所述辛烷值助剂包含有机金属辛烷值助剂。
7.如权利要求6所述的减少颗粒物排放量的方法，其中所述有机金属辛烷值助剂包含锰，并且其中所述有机金属辛烷值助剂的量足以使得所述燃料制剂每升包含按重量计至少5ppm的锰。
8.如权利要求6所述的减少颗粒物排放量的方法，其中所述燃料制剂每升包含按重量计至少10ppm的锰。
9.如权利要求6所述的减少颗粒物排放量的方法，其中所述有机金属辛烷值助剂包含铁，并且其中所述有机金属辛烷值助剂的量足以使得总的火花点火燃料制剂每升包含按重量计至少5ppm的铁。
10.如权利要求9所述的减少颗粒物排放量的方法，其中所述总的火花点火燃料制剂每升包含按重量计至少10ppm的铁。
11.如权利要求6所述的减少颗粒物排放量的方法，其中所述有机金属辛烷值助剂包括甲基环戊二烯三羰基锰。
12.一种内燃机燃料制剂，其包含：
含有最多为ppm硫的燃料；所述燃料的芳烃含量为至少约20体积％；
辛烷值助剂，其中所述燃料的研究法辛烷值为至少85；
其中所述燃料的T90为至少140℃；和
其中产生于所述燃料制剂在发动机中燃烧的颗粒物排放量减少了，与包括增多量的芳烃作为所述辛烷值助剂替代物的可比燃料制剂的燃烧相比。
13.配制火花点火燃料的方法，包括以下步骤：
提供基础燃料，所述基础燃料的芳烃含量为所述基础燃料的至少10体积％；
通过添加包含辛烷值助剂的添加剂混合物配置成品燃料，其中所述添加剂混合物还具有小于约2％的芳烃含量；
其中，在所述成品燃料燃烧之后，其颗粒物排放数小于来自所述基础燃料燃烧的颗粒数。
14.由内燃机产生的尾喷焰，其具有：
固体颗粒数排放率小于约6X1012#/km，根据新欧洲行驶循环和颗粒物测量程序测量方法测得；
其中在产生所述尾喷焰的内燃机中燃烧的燃料包括辛烷值助剂、少于50ppm的硫、至少10体积％的芳烃、以及T90为至少约140℃。
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| US14/516,627 US9587190B2 (en) | 2014-10-17 | 2014-10-17 | Fuel composition and method of formulating a fuel composition to reduce real-world driving cycle particulate emissions |
| PCT/US2015/055221 WO2016061035A1 (en) | 2014-10-17 | 2015-10-13 | Fuel composition and method of formulating a fuel composition to reduce real-world driving cycle particulate emissions |
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| Publication number | Publication date |
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| AU2015333772B2 (en) | 2018-03-15 |
| US9587190B2 (en) | 2017-03-07 |
| AU2015333772A1 (en) | 2017-04-27 |
| RU2679143C2 (ru) | 2019-02-06 |
| US20160108332A1 (en) | 2016-04-21 |
| BR112017007398B1 (pt) | 2018-10-23 |
| EP3207109A1 (en) | 2017-08-23 |
| WO2016061035A1 (en) | 2016-04-21 |
| CN106795445B (zh) | 2019-09-13 |
| MX2017004835A (es) | 2017-08-15 |
| CA2963430A1 (en) | 2016-04-21 |
| BR112017007398A2 (pt) | 2017-10-17 |
| RU2017117002A (ru) | 2018-11-19 |
| EP3207109A4 (en) | 2018-05-02 |
| CA2963430C (en) | 2022-10-18 |
| EP3207109B1 (en) | 2021-12-08 |
| RU2017117002A3 (zh) | 2018-11-19 |
| CL2017000947A1 (es) | 2018-01-05 |
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