CN112789346A - 负氢离子供体作为减少低速早燃事件的添加剂 - Google Patents
负氢离子供体作为减少低速早燃事件的添加剂 Download PDFInfo
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- CN112789346A CN112789346A CN201980065359.8A CN201980065359A CN112789346A CN 112789346 A CN112789346 A CN 112789346A CN 201980065359 A CN201980065359 A CN 201980065359A CN 112789346 A CN112789346 A CN 112789346A
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- Prior art keywords
- hydrogen ion
- negative hydrogen
- internal combustion
- based reducing
- agents
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- BOPGDPNILDQYTO-NNYOXOHSSA-N nicotinamide-adenine dinucleotide Chemical compound C1=CCC(C(=O)N)=CN1[C@H]1[C@H](O)[C@H](O)[C@@H](COP(O)(=O)OP(O)(=O)OC[C@@H]2[C@H]([C@@H](O)[C@@H](O2)N2C3=NC=NC(N)=C3N=C2)O)O1 BOPGDPNILDQYTO-NNYOXOHSSA-N 0.000 description 7
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- XFXPMWWXUTWYJX-UHFFFAOYSA-N Cyanide Chemical group N#[C-] XFXPMWWXUTWYJX-UHFFFAOYSA-N 0.000 description 2
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- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 description 2
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- 239000003879 lubricant additive Substances 0.000 description 2
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- WKBOTKDWSSQWDR-UHFFFAOYSA-N Bromine atom Chemical compound [Br] WKBOTKDWSSQWDR-UHFFFAOYSA-N 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 1
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- GDTBXPJZTBHREO-UHFFFAOYSA-N bromine Substances BrBr GDTBXPJZTBHREO-UHFFFAOYSA-N 0.000 description 1
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- TVMXDCGIABBOFY-UHFFFAOYSA-N octane Chemical compound CCCCCCCC TVMXDCGIABBOFY-UHFFFAOYSA-N 0.000 description 1
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- ISWSIDIOOBJBQZ-UHFFFAOYSA-N phenol group Chemical group C1(=CC=CC=C1)O ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 1
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- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 description 1
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Classifications
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
- C10M133/00—Lubricating compositions characterised by the additive being an organic non-macromolecular compound containing nitrogen
- C10M133/02—Lubricating compositions characterised by the additive being an organic non-macromolecular compound containing nitrogen having a carbon chain of less than 30 atoms
- C10M133/38—Heterocyclic nitrogen compounds
- C10M133/40—Six-membered ring containing nitrogen and carbon only
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L1/00—Liquid carbonaceous fuels
- C10L1/10—Liquid carbonaceous fuels containing additives
- C10L1/14—Organic compounds
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L1/00—Liquid carbonaceous fuels
- C10L1/04—Liquid carbonaceous fuels essentially based on blends of hydrocarbons
- C10L1/06—Liquid carbonaceous fuels essentially based on blends of hydrocarbons for spark ignition
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L1/00—Liquid carbonaceous fuels
- C10L1/04—Liquid carbonaceous fuels essentially based on blends of hydrocarbons
- C10L1/08—Liquid carbonaceous fuels essentially based on blends of hydrocarbons for compression ignition
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L1/00—Liquid carbonaceous fuels
- C10L1/10—Liquid carbonaceous fuels containing additives
- C10L1/14—Organic compounds
- C10L1/22—Organic compounds containing nitrogen
- C10L1/222—Organic compounds containing nitrogen containing at least one carbon-to-nitrogen single bond
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L10/00—Use of additives to fuels or fires for particular purposes
- C10L10/10—Use of additives to fuels or fires for particular purposes for improving the octane number
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L10/00—Use of additives to fuels or fires for particular purposes
- C10L10/12—Use of additives to fuels or fires for particular purposes for improving the cetane number
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
- C10M127/00—Lubricating compositions characterised by the additive being a non- macromolecular hydrocarbon
- C10M127/04—Lubricating compositions characterised by the additive being a non- macromolecular hydrocarbon well-defined aromatic
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Abstract
提供了包含有机负氢离子基还原剂的燃料和润滑剂组合物。还提供了使用这些组合物防止或减少内燃机中低速早燃事件的方法。
Description
技术领域
本公开涉及燃料和润滑剂组合物以及使用该组合物降低内燃机中的低速早燃活度的方法。所述组合物包括有机负氢离子供体作为燃料或润滑剂添加剂。
背景
内燃发动机中的早燃是不希望的事件，其中在空气燃料混合物的期望点火之前(例如通过火花塞)发生了空气燃料混合物的不期望的点火。在高负荷发动机运转期间，早燃可能是一个问题，因为来自发动机运转的热量可能会将燃烧室的一部分加热到足以在接触时点燃空气燃料混合物的温度。
近年来，发动机制造商已经开发出较小的发动机，其可提供更高的功率密度和出色的性能，同时减少摩擦和泵送损失。这种性能的改进通过使用涡轮增压器或机械增压器提高增压压力完成，以及通过使用由在较低发动机速度下产生的较高扭矩所允许的更高的传动齿轮比来使发动机减速而实现。不利之处在于这些发动机通常在低速和高负荷驾驶条件下运行，从而使发动机更容易受到称为随机早燃或低速早燃(LSPI)的早燃现象的影响。在最坏的情况下，极高的汽缸峰值压力会累积并导致灾难性的发动机故障。这种敏感性使发动机制造商无法在这种较小的高输出发动机中以较低的发动机转速充分优化发动机扭矩。
概要
一方面，提供了一种燃料组合物，所述燃料组合物包含(1)大于50重量％沸点在汽油或柴油范围内的烃燃料以及(2)少量的一种或多种有机负氢离子基还原剂。
在另一方面，提供了一种用于防止或减少内燃发动机中的低速早燃事件的方法，所述方法包括向发动机供应燃料组合物，所述燃料组合物包括(1)大于50重量％沸点在汽油或柴油范围内的烃燃料以及(2)少量的一种或多种有机负氢离子基还原剂。
在另一方面，提供了一种润滑油组合物，所述润滑油组合物包含(1)大于50重量％基础油以及(2)少量的一种或多种有机负氢离子基还原剂。
在又一方面，提供了一种用于防止或减少火花点火式内燃机中的低速早燃事件的方法，所述方法包括向发动机供应润滑油组合物，所述润滑油组合物包含(1)大于50重量％基础油以及(2)少量的一种或多种有机负氢离子基还原剂。
详细说明
定义
在本说明书中，如果使用以下词语和表达，则其具有如下含义。
术语“增压”是指在比自然吸气发动机更高的吸入压力下运行发动机。增压的条件可以通过使用涡轮增压器(由排气驱动)或增压器(由发动机驱动)来达到。“增压”使发动机制造商可以使用较小的发动机，这些发动机可以提供更高的功率密度，以提供出色的性能，同时减少摩擦和泵送损失。
术语“油溶性”是指对于给定的添加剂，可以通过溶解、分散或悬浮在具有润滑粘度的油中来掺入以提供所需活性或性能水平所需的量。通常，通常，这意味着可以将至少0.001重量％的添加剂掺入润滑油组合物中。术语“可溶于燃料的”是添加剂溶解、分散或悬浮在燃料中的类似表达。
“汽油”或“汽油沸程组分”是指包含至少主要为C4-C12烃的组合物。在一个实施方案中，将汽油或汽油沸程范围组分进一步定义为是包含至少主要为C4-C12烃并且进一步的沸程为约37.8℃(100°F)至约204℃(400°F)的组合物。在一个替代实施方案中，汽油或汽油沸程范围组分被定义为包含至少主要为C4-C12烃，其沸程为37.8℃(100°F)至约204℃(400°F)，并进一步定义为符合ASTM D4814的组合物。
术语“柴油”是包含至少主要为C10-C25烃的中间馏分燃料。在一个实施方案中，柴油被进一步定义为是指包含至少主要为C10-C25烃并且进一步沸程为约165.6℃(330°F)至约371.1℃(700°F)的组合物。在一个替代实施方案中，柴油如上所定义，是指包含至少主要为C10-C25烃，其沸程为约165.6℃(330°F)至约371.1℃(700°F)，并且进一步定义为符合ASTM D975的组合物。
术语“烷基”是指饱和的烃基，其可以是直链、支链、环状或环状、直链和/或支链的组合。
“次要量”是指小于组合物的50重量％，以相对于所述添加剂和相对于组合物的总重量表示，被认为是添加剂的活性成分。
“还原剂”是在氧化还原反应中向另一个化学物质提供电子的还原剂，“负氢离子基还原剂”在氧化还原反应中向另一个化学物质提供一个负氢离子(氢的阴离子)。
在基于烃的配方(特别是润滑剂)的上下文中，术语“灰分”是指在烃已经煅烧之后残留的金属化合物。该灰分主要来源于某些添加剂中使用的化学物质以及固体。术语“无灰”是指不产生灰分或不限制灰分生成的配方或添加剂。无灰添加剂通常不含金属(包括硼)、硅、卤素，或以低于典型仪器检测极限的浓度包含这些元素。
“卤素”是各个取代基的统称，包括例如氟、氯、溴、碘等。
“类似物”是具有与另一种化合物相似的结构但在某些部分上不同的化合物，例如一个或多个原子、官能团、亚结构，其被其他原子、基团或亚结构取代。
“同系物”是指由重复单元彼此不同的一系列化合物组成的化合物。烷烃是同系物的例子。例如，乙烷和丙烷是同系物，因为它们仅在重复单元(-CH2-)的长度上有所不同。同系物可以被认为是特定类型的类似物。
“衍生物”是通过化学反应(例如，酸碱反应、氢化等)从相似化合物衍生的化合物，在取代基的情况下，衍生物可以是一个或多个部分的组合。例如，酚部分可以被认为是芳基部分和羟基部分的衍生物，相关领域的普通技术人员会知道什么被认为是衍生物的边界和界限。
“发动机”或“燃烧发动机”是燃料的燃烧在燃烧室内发生的热力发动机。“内燃机”是在有限的空间(“燃烧室”)中发生燃料燃烧的热力发动机。“火花点火发动机”是燃烧通常由火花(通常是火花塞)点燃的热力发动机，这与“压燃式发动机”(通常为柴油发动机)形成对比，在这种发动机中，压缩产生的热量与燃油喷射足以在没有外部火花下启动燃烧。
介绍
低速早燃(LSPI)的一种可能原因是在发动机低速运行且压缩冲程时间最长的期间，高压下从活塞缝隙进入发动机燃烧室的发动机油滴自动点火。诸如涡轮增压器的使用、发动机设计、发动机涂层、活塞形状、燃料选择或发动机机油添加剂等因素可能会导致LSPI事件的增加。尽管可以通过使用新发动机技术或优化发动机工况来解决某些发动机爆震和早燃问题，但通过新的燃料和/或润滑油组合物降低LSPI可能是最经济的方法。
本公开内容描述了基于烃的组合物(例如，燃料、润滑油)及其使用方法，其中所述基于烃的组合物在内燃机运转期间防止LSPI事件或降低LSPI活性。合适的基于烃的组合物将具有根据本公开的有机负氢离子基还原剂添加剂。
有机负氢离子基还原剂
本文提供了防止燃烧发动机中的LSPI事件或降低LSPI活性的有机负氢离子基还原剂。这些有机负氢离子基还原剂是在负氢离子转移步骤中易于提供负氢离子的有机分子。这些还原剂是无灰的添加剂，通常含有碳、氢、氮和/或氧原子。根据应用，有机负氢离子基还原剂是油溶性或燃料溶性的。
负氢离子转移是许多著名的有机反应(包括重要的生化反应和工业氧化还原反应)中的关键步骤。在这些类型的反应中，还原剂会提供负氢离子(H-)转移到底物上，例如羰基化合物、二氧化碳、亚胺、含有活性C═C键的化合物等。负氢离子转移的精确机理通常很复杂，并且可能随温度、底物、负氢离子供体、质子的可用性、路易斯酸的存在等而变化。在某些情况下，负氢离子转移可通过将负氢离子从负氢离子供体直接转移至基质而进行，或可在连续步骤中发生(例如，电子转移至基质，接着是氢原子或质子和第二电子)。
不受理论的限制，据信根据本发明的合适的负氢离子供体可通过对抗可引发LSPI事件的氧化不稳定化学物质起作用而降低内燃机中的LSPI活性。这可能涉及将氧化不稳定的化学物质还原为更稳定、反应性较低的还原物质，从而抑制LSPI事件。
据本发明的一个或多个实施方案，所述有机负氢离子基还原剂包括以下有机负氢离子供体中的至少一种：二氢吡啶(DHPD)、还原态烟酰胺腺嘌呤二核苷酸(NADH)、亚甲基四氢甲蝶呤、吖啶、三芳基甲烷、三胺、芳基苯并咪唑啉、二氧戊环、二醚环己二烯、环庚三烯、黄素腺嘌呤二核苷酸(FADH2)，六氢三氮杂萘、其类似物、其同系物及其衍生物。
提供以下有机负氢离子基还原剂的化学结构用于说明。每种还原剂或还原剂类型均由通用结构表示，该通用结构在各个取代位置上包括上位R基团(例如，R1,R2,R3,等)。每个R基团可以是选自一组合适的取代基的成员。改变R基团取代基的组合可以产生一组相关结构，其中每个所得结构是该组内其他结构的类似物。基团取代基的期望性可取决于许多因素，包括但不限于有机负氢离子基供体的提供负氢离子的目标能力、稳定性、在油或燃料中的溶解度等。
二氢吡啶(DHPD)
DHPD或DHPD型还原剂由通用结构(式1)说明。参考式1，R1、和R2是各自独立地选自以下组的成员：H、酯部分、酰胺部分、氰化物部分、其任意衍生物等。R3和R4是各自独立地选自以下组的成员：H、烷基部分、其任意衍生物等。R5是选自以下组的成员：H、烷基部分、烯丙基部分、芳基部分、苄基部分、链烷醇部分、其任意衍生物等。
DHPD的合适类似物包括
还原态烟酰胺腺嘌呤二核苷酸(NADH)
NADH或NADH型还原剂由通用结构(式2)说明。参考式2，R1和R2是各自独立地选自以下组的成员：H、酯部分、酰胺部分、氰化物部分、其任意衍生物等。R3和R4是各自独立地选自以下组的成员：H、烷基部分、其任意衍生物等。R5是选自以下组的成员：H、烷基部分、烯丙基部分、芳基部分、苄基部分、链烷醇部分、其任意衍生物等。R6选自以下组的成员：H、烷基部分、其任意衍生物等。在一些实施方案中，R1和R3或R1和R4可以形成环状结构(例如，式2C和2E)。
NADH的合适类似物包括
亚甲基四氢甲蝶呤
亚甲基四氢甲基蝶呤或亚甲基四氢甲基蝶呤型还原剂由通用结构(式3)表示。参考式3，R1、R2、R3和R4是各自独立地选自以下组的成员：H、烷基部分、烯丙基部分、链烷醇部分、其任意衍生物等。R5选自以下组：H、烷基部分、其任意衍生物等。
亚甲基四氢甲蝶呤的合适类似物包括
吖啶
吖啶或吖啶型还原剂由通用结构(式4)说明。参考式4，X为N或O(式4H)。当X为N时，R1选自以下的组：H、烷基部分、烯丙基部分、芳基部分、苄基部分、其任意衍生物等。R2选自以下的组：H、烷基部分、烯丙基部分、芳基部分、苄基部分、链烷醇部分、其任意衍生物等。R3和R4是各自独立地选自以下组的成员：H、烷基部分、芳基部分、苄基部分、胺部分、烷氧基部分、杂原子、其任意衍生物等。而且，R3以及R4可以独立地在其各自的环内占据一个以上的取代位置。在一些实施方案中，R1和R3或R1和R4可以形成环状结构(例如，式4E和4F)。
吖啶的合适类似物包括
三芳基甲烷
三芳基甲烷或三芳基甲烷型还原剂由通用结构(式5)说明。参考式5，R1、R2和R3是各自独立地选自以下组：H，烷基部分、芳基部分、苄基部分、烯丙基部分、酰胺部分、酯部分、醚部分、羟基部分、胺部分、其任意衍生物等。在一些实施方案中，R1、R2和R3可以独立地在其各自的环内占据一个以上的取代位置(例如，式5A和5B)。
三芳基甲烷的合适类似物包括
三胺
三胺或三胺型还原剂由通用结构(式6)说明，其中R1、R2、R3、R4、R5、和R6连接成三个环(例如，式6A至6C)。
三胺的合适类似物包括
芳基苯并咪唑啉
芳基苯并咪唑啉或芳基苯并咪唑啉型还原剂由通用结构(式7)说明。参考式7，X为N、O或S。如果X为N，R1和R2是各自独立地选自以下组的成员：H、烷基部分、其任意衍生物等。R3选自以下组：H、烷基部分，烯烃部分、炔烃部分、芳基部分、苄基部分、其任意衍生物等。R4选自以下组：H、烷基部分、芳基部分、苄基部分、烯丙基部分、其任意衍生物等。在一些实施方案中，R4可独立地占据一个以上取代位置。
芳基苯并咪唑啉的合适类似物包括
二氧戊环
二氧戊环或二氧戊环型还原剂由通用结构(式8)说明。参考式8，R是选自以下组的成员：H、烷基部分、烯丙基部分、苄基部分、链烷醇部分、其任意衍生物等。
二氧戊环的合适类似物包括
二醚环己二烯
二醚环己二烯或二醚环己二烯型还原剂由通用结构(式9)说明。参考式9，R是选自以下组的成员：H、烷基部分、烯丙基部分、苄基部分、链烷醇部分、其任意衍生物等。
二醚环己二烯的合适类似物包括
环庚三烯
环庚三烯或环庚三烯型还原剂由通用结构(式10)说明。参考式10，R是选自以下组的成员：H、烷基部分、烯丙基部分、苄基部分、链烷醇部分、其任意衍生物等。在一些实施方案中，R可独立地占据一个以上取代位置(例如，式10B)。
环庚三烯的合适类似物包括
本文所述的负氢离子供体可以是合成的或购自化学品供应商。提供以下实施例仅用于说明性目的，而无意于限制本发明。DHPD和DHPD型还原剂可通过利用以不同的1,4二氢吡啶酰胺形式的可关开的可转化的酰基供体方案合成(Org.Biomol.Chem.2015,13,185-198)。二甲基3，5-二羧酸吡啶可以从Sigma-Aldrich(St.Louis,MO)购买，或通过已知方法制备(J.Am.Chem.Soc.2000,122,9014-9018)。式6A可以通过已知的方案(Syn.Comm.1994,24,3109-3114)合成。对甲氧基苯苯并咪唑啉或对叔丁基苯苯并咪唑啉可采用已知的合成方法获得(Syn.Comm.1983,13,1033-1039)。可以通过采用已知的合成方法来获得式2F(Org.Lett.2013,15,180-183)。
燃料组合物
本公开的有机负氢离子基供体可用作烃燃料中的添加剂，以防止或减少内燃机中的不期望的点火事件。当用于燃料中时，为实现所需的LSPI降低或功效所必需的添加剂的适当浓度取决于多种因素，包括所用燃料的类型、其他清净剂或分散剂或其他添加剂的存在等。本发明的添加剂在烃类燃料中的浓度范围可以为以重量计25至5000重量份/百万(ppmw)(包括但不限于50至4000ppm、100至3500、150至3000、200到2500、250到2000、300到1500、350到1000等)。如果燃料组合物中存在其他负氢离子供体，则可以使用较少量的添加剂。
在一些实施方案中，可以使用在65℃至205℃范围内沸腾的惰性稳定的亲油性(即，可溶于烃燃料中)有机溶剂将本公开的化合物配制成浓缩物。可以使用脂肪族或芳族烃溶剂，例如苯、甲苯、二甲苯或更高沸点的芳族化合物或芳族稀释剂。含有2至8个碳原子的脂肪醇，例如乙醇、异丙醇、甲基异丁基甲醇、正丁醇等，与烃类溶剂结合，也适合与本发明的添加剂一起使用。在浓缩物中，添加剂的量可以在10至70重量％的范围内(例如20至40重量％)。
在汽油或汽油燃料中，可以使用其他众所周知的添加剂，包括含氧化合物(例如乙醇、甲基叔丁基醚)，其他抗爆剂和清净剂/分散剂(例如烃基胺、烃基聚(氧化烯)胺、琥珀酰亚胺、曼尼希反应产物、聚烷基苯氧基烷醇的芳族酯或聚烷基苯氧基氨基烷烃)。另外，可以存在摩擦改进剂、抗氧化剂、金属减活剂和破乳剂。
在柴油燃料中，可以使用其他公知的添加剂，例如降凝剂、流动改进剂、十六烷值改进剂、润滑性添加剂等。
燃料可溶的、不挥发的载体流体或油也可与本公开的化合物一起使用。载体流体是化学惰性的烃溶性液体媒介物，其显著增加了燃料添加剂组合物的非挥发性残余物(NVR)或无溶剂液体部分，同时又不致于导致辛烷需求的增加。载体流体可以是天然油或合成油，例如矿物油、精制石油、合成聚烷烃和烯烃，包括氢化和未氢化的聚α-烯烃、合成聚氧化烯衍生的油，例如美国专利Nos.3,756,793；4,191,537；和5,004,478；以及欧洲专利申请公开Nos.356,726和382,159中描述的那些。
载体流体的使用量可以为烃燃料重量的35-5000ppm(例如，燃料的50-3000ppm)。当用于燃料浓缩物中时，载体流体可以以20至60重量％的量存在(例如30至50重量％)。
润滑油组合物
本公开的有机负氢离子供体可用作润滑油中的添加剂，以防止或减少内燃机中不期望的点火事件。当以这种方式使用时，添加剂在润滑油组合物中的浓度通常为0.001-10重量％，基于润滑油组合物的总重量(包括但不限于0.01至5重量％、0.2至4重量％、0.5至3重量％、1至2重量％等)。如果在润滑油组合物中存在其他负氢离子供体，则可以使用较少量的添加剂。
将根据所需的最终用途和成品油中的添加剂选择或掺混用作基础油的油，以得到所需等级的机油，例如具有汽车工程师协会(SAE)粘度等级0W,0W-20、0W-30、0W-40、0W-50、0W-60、5W、5W-20、5W-30、5W-40、5W-50、5W-60、10W、10W-20、10W-30、10W-40、10W-50、15W、15W-20、15W-30、或15W-40的润滑油组合物。
具有润滑粘度的油(有时称为“基础油料”或“基础油”)是润滑剂的主要液体成分，将添加剂和可能的其他油混入其中，例如可制成成品润滑剂(或润滑剂组合物)。可用于制备浓缩物以及由其制备润滑油组合物的基础油可选自天然(植物、动物或矿物)和合成润滑油及其混合物。
本公开中的基础油和基础油的定义与在美国石油协会(API)出版物1509附件E(“API Base Oil Interchangeability Guidelines for Passenger Car Motor Oils andDiesel Engine Oils”，2016年12月)中的定义相同。使用表E-1中指定的测试方法，第I类基础油料中的饱和物含量小于90％和/或硫含量大于0.03％，粘度指数大于或等于80且小于120。使用表E-1中指定的测试方法，第II类基础油料中的饱和物等于或大于90％且硫含量小于或等于0.03％，粘度指数大于或等于80且小于120。使用表E-1中指定的测试方法，第III类基础油料中的饱和物大于或等于90％且硫含量小于或等于0.03％，粘度指数大于或等于120。第IV类基础油料是聚α烯烃(PAO)。第V类基础油料包括所有其他第I、II、III或IV类中未包括的其他基础油料。
天然油包括动物油、植物油(例如，蓖麻油和猪油)和矿物油。可以使用具有良好的热氧化稳定性的动植物油。在天然油中，优选矿物油。矿物油的原油来源差异很大，例如，它们是链烷烃、环烷烃还是混合链烷烃-环烷烃。衍生自煤或页岩的油也是有用的。天然油的生产和纯化方法也有所不同，例如，其蒸馏范围以及是直馏还是裂化、加氢精制或溶剂萃取。
合成油包括烃油。烃油包括诸如聚合和共聚的烯烃(例如，聚丁烯、聚丙烯、丙烯异丁烯共聚物、乙烯-烯烃共聚物和乙烯-α-烯烃共聚物)的油。聚α烯烃(PAO)油基础油料是常用的合成烃油。举例来说，衍生自C8到C14烯烃PAOs，例如可以使用C8、C10、C12、C14烯烃或其混合物。
其他用作基础油的有用流体包括非常规基础油料，它们已经过加工，优选经过催化或合成后可提供高性能特性。
非常规基础油/基础油料包括一种或多种衍生自一种或多种气制液(GTL)物质的基础油混合物，以及衍生自天然蜡或蜡状进料的异构体/异蜡脱蜡基础油、矿物蜡或非矿物油蜡状原料，例如散蜡、天然蜡，以及蜡质原料，例如瓦斯油、蜡状燃料加氢裂化底部馏分、蜡状提余油、加氢裂化油、热裂化油或其他矿物、矿物油、甚至是非石油衍生的蜡质物质，例如从煤液化或页岩油中获得的蜡质物质，以及这些基础油的混合物。
用于本公开的润滑油组合物中的基础油是对应于API第I类、第II类、第III类、第IV类、和第V类油的各种油中的任何一种，及其混合物，优选API第II类、第III类、第IV类、和第V类油，以及它们的混合物，更优选的是第III至V类基础油，因为它们具有出色的挥发性、稳定性、粘度和清洁度特征。
通常，基础油在100℃下的运动粘度(ASTM D445)为2.5至20mm2/s(例如3到12mm2/s、4至10mm2/s、或4.5至8mm2/s)。
本发明的润滑油组合物还可以包含常规的润滑剂添加剂，以赋予辅助功能，以得到成品润滑油组合物，其中这些添加剂被分散或溶解。例如，可以将润滑油组合物与抗氧化剂、无灰分散剂、抗磨剂、清净剂如金属清净剂、防锈剂、除雾剂、破乳剂、摩擦改性剂、金属减活剂、降凝剂、粘度调节剂、消泡剂、助溶剂、包装增容剂、缓蚀剂、染料、极压剂等及其混合物。多种添加剂是已知的并且可商购。这些添加剂或它们的类似化合物可以通过常规的混合方法用于制备本发明的润滑油组合物。
当使用时，每种前述添加剂以功能有效量使用以赋予润滑剂所需的性能。因此，例如，如果添加剂是无灰分散剂，则该无灰分散剂的功能有效量将是足以赋予润滑剂所需的分散性的量。通常，除非另外指明，否则这些添加剂中的每一种的浓度可以在约0.001至约20重量％的范围内，例如约0.01至约10重量％。
实施例
以下说明性示例旨在是非限制性的。
虽然LSPI可以影响许多类型的内燃机，但在直喷、增压(涡轮增压或增压)、火花点火(汽油)内燃机中运行时，其在1500至2500转/分钟(rpm)的发动机转速下(例如在1500至2000rpm的发动机转速下)，产生的制动平均有效压力水平大于1000kPa(10bar)。制动平均有效压力(BMEP)定义为在发动机循环期间完成的功除以发动机排量，通过发动机排量归一化的发动机扭矩。“制动”一词表示在测功机上测得的发动机飞轮上的实际扭矩或功率，因此BMEP是对发动机有用能量输出的量度。
现已发现，本公开的燃料组合物或润滑油组合物可以防止或最小化内燃机中的早燃问题。
实施例1-8
将测试化合物掺入汽油或润滑油中，并使用以下描述的测试方法确定其降低LSPI事件的能力。
将通用汽车(GM)2.0L LHU 4-缸汽油涡轮增压直喷式发动机用于LSPI测试。每个汽缸装备有燃烧压力传感器。
使用六段测试程序来测定在2000rpm的发动机速度和275Nm的负荷条件下发生的LSPI事件的数目。LSPI测试条件运行28分钟，并且每段通过空转时段隔开。每段被稍微截断(truncated)以消除瞬态部分。每个截断的段典型地具有大致110000个燃烧循环(27500个燃烧循环/汽缸)。总之，六个截断的段具有大致660000个燃烧循环(165000个燃烧循环/汽缸)。
LSPI影响的燃烧循环通过监测在5％总热释放(AI5)的曲轴转角和峰值汽缸压力(PP)来测定。LSPI影响的燃烧循环定义为具有(1)对于给定的汽缸和截断段，PP比平均PP大五个标准偏差，和(2)对于给定的汽缸和截断段，AI5比平均大了五个标准偏差。
LSPI频率作为LSPI影响的燃烧循环的数目/百万个燃烧循环来报告，并且如下计算：
LSPI频率＝[(六个截断的段中LSPI影响的燃烧循环的总数)/(六个截断的段中燃烧循环的总数)]×1000000
当与相应的基准燃料和/或基准润滑剂相比时，与降低了LSPI频率的测试燃料和/或测试润滑剂相关的添加剂被认为是减轻LSPI频率的添加剂。为了在此进行测试，基准燃料是不含任何沉积物控制添加剂的常规49国家优质无铅汽油燃料，并且基准润滑剂代表了满足ILSAC GF-5和API SN规范的常规发动机油。测试结果列于表1。
实施例总结了各种燃料或润滑油添加剂的测试结果。例如，实施例1示出了在测试燃料流体中DHPD作为燃料添加剂在1000ppmw下的结果。在标题为“LSPI活性”的列中列出了测试含添加剂的燃料或润滑剂时观察到的LSPI事件的数目，而标题为“参比”的列中列出了在测试不含添加剂的燃料或润滑剂时观察到的LSPI事件的数目。对于给定的示例，添加剂的包含或省略是LSPI活性和参比列中测试的燃料或润滑剂成分之间的唯一区别。
Claims (20)
1.一种燃料组合物，所述燃料组合物包括(1)大于50重量％沸点在汽油或柴油范围内的烃燃料以及(2)少量的一种或多种有机负氢离子基还原剂。
2.根据权利要求1所述的燃料组合物，其中所述有机负氢离子基还原剂基本不含卤素、硼或硅。
3.根据权利要求1所述的燃料组合物，其中所述有机负氢离子基还原剂是二氢吡啶、烟酰胺腺嘌呤二核苷酸、亚甲基四氢甲蝶呤、吖啶、三芳基甲烷、六氢三氮杂苯并菲、三胺、芳基苯并咪唑啉、二氧戊环、二醚环己二烯、环庚三烯、黄素腺嘌呤二核苷酸或其类似物。
4.根据权利要求1所述的燃料组合物，其中所述有机负氢离子基还原剂的存在量为以重量计25至5000ppm。
5.根据权利要求1所述的燃料组合物，其中所述有机负氢离子基还原剂的存在量为以重量计250至2000ppm。
6.根据权利要求1所述的燃料组合物，进一步包括：
含氧化合物、抗爆剂、清净剂、分散剂、摩擦改进剂、抗氧化剂、金属减活剂、破乳剂、降凝剂、流动改进剂、十六烷值改进剂或润滑性添加剂。
7.一种防止或减少内燃机中不期望的点火事件的方法，所述方法包括：
向所述发动机供应燃料组合物，所述燃料组合物包含(1)大于50重量％沸点在汽油或柴油范围内的烃燃料以及(2)少量的一种或多种有机负氢离子基还原剂。
8.根据权利要求7所述的方法，其中所述内燃机是火花点火式。
9.根据权利要求7所述的方法，其中所述内燃机在小于3000rpm下运行。
10.根据权利要求7所述的方法，其中所述火花点火式内燃发动机在制动平均有效压力至少为1MPa(10bar)的负荷下运行。
11.一种润滑油组合物，所述润滑油组合物包括(1)大于50重量％基础油以及(2)少量的一种或多种有机负氢离子基还原剂。
12.根据权利要求11所述的润滑油组合物，其中所述有机负氢离子基还原剂基本不含卤素、硼或硅。
13.根据权利要求11所述的润滑油组合物，其中所述有机负氢离子基还原剂是二氢吡啶、烟酰胺腺嘌呤二核苷酸、亚甲基四氢甲蝶呤、吖啶、三芳基甲烷、六氢三氮杂苯并菲、三胺、芳基苯并咪唑啉、二氧戊环、二醚环己二烯、环庚三烯、黄素腺嘌呤二核苷酸或其类似物。
14.根据权利要求11所述的润滑油组合物，其中所述有机负氢离子基还原剂的存在量为0.001至10重量％。
15.根据权利要求11所述的润滑油组合物，其中所述有机负氢离子基还原剂的存在量为0.5至5重量％。
16.根据权利要求11所述的润滑油组合物，进一步包括：
抗氧化剂、无灰分散剂、抗磨剂、清净剂、防锈剂、除雾剂、破乳剂、摩擦改进剂、金属减活剂、降凝剂、粘度调节剂、消泡剂、助溶剂、包装增容剂、缓蚀剂、染料或极压剂。
17.一种防止或减少内燃机中不期望的点火事件的方法，所述方法包括：
向所述发动机供应润滑油组合物，所述润滑油组合物包含(1)大于50重量％基础油以及(2)少量的一种或多种有机负氢离子基还原剂。
18.根据权利要求17所述的方法，其中所述内燃机是火花点火式。
19.根据权利要求17所述的方法，其中所述内燃机在小于3000rpm下运行。
20.根据权利要求17所述的方法，其中所述内燃发动机在制动平均有效压力至少为1MPa(10bar)的负荷下运行。
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| PCT/IB2019/058397 WO2020070672A1 (en) | 2018-10-04 | 2019-10-02 | Hydride donors as an additive for reducing low speed pre-ignition events |
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| KR20210069064A (ko) | 2021-06-10 |
| EP3861089A1 (en) | 2021-08-11 |
| US20200109343A1 (en) | 2020-04-09 |
| WO2020070672A1 (en) | 2020-04-09 |
| MX2021003690A (es) | 2021-06-04 |
| ZA202102156B (en) | 2022-09-28 |
| AU2019353900A1 (en) | 2021-05-06 |
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