CN101072855B - 用多重抗氧化剂稳定的润滑剂组合物 - Google Patents
用多重抗氧化剂稳定的润滑剂组合物 Download PDFInfo
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- CN101072855B CN101072855B CN2005800420172A CN200580042017A CN101072855B CN 101072855 B CN101072855 B CN 101072855B CN 2005800420172 A CN2005800420172 A CN 2005800420172A CN 200580042017 A CN200580042017 A CN 200580042017A CN 101072855 B CN101072855 B CN 101072855B
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Abstract
公开了润滑剂组合物,该组合物包含润滑油和至少两种抗氧化剂的混合物,其中第一抗氧化剂是仲二芳基胺,第二抗氧化剂是取代的对亚苯基二胺。还公开了提高润滑油的氧化稳定性的方法,该方法包括向所述润滑油中添加至少两种抗氧化剂,其中第一抗氧化剂是仲二芳基胺,第二抗氧化剂是取代的对亚苯基二胺。
Description
我们根据Title35,United States Code,§120要求于2004年12月10日提交的标题为“用多重抗氧化剂稳定的润滑剂组合物”的美国临时申请号60/634,535的权益。
发明背景
1.技术领域
本发明涉及通过向润滑剂,尤其是烃基润滑油中添加仲二芳基胺和取代的对亚苯基二胺的组合物改进所述润滑剂的氧化稳定性。
2.相关技术的描述
润滑剂,如在各种机器中使用的那些,在储存、运输和使用期间对氧化变质敏感,当此类润滑剂暴露于高温和铁催化环境下时尤其如此,这大大地促进了它们的氧化。这种氧化如果不加以控制会导致腐蚀性的酸性产物、淤渣、油漆、树脂和其它不溶于油的产物形成,并可能引起润滑剂的设定的物理和摩擦性能损失。因此常用的做法是将抗氧化剂加入润滑剂以防止(至少在某种程度上)氧化,从而延长它们的使用寿命。包含各种仲二芳基胺作为抗氧化剂的润滑剂组合物在本领域中是公知的。使用对亚苯基二胺也是已知的,尽管程度上更小。
美国专利号2,451,642公开了对亚苯基二胺作为润滑油组合物的有用的抗氧化剂,所述润滑油组合物用于其中可能发生铁催化氧化反应的环境。
美国专利号2,718,501公开了由芳族胺和有机脂族含硫化合物构成的稳定剂体系,所述芳族胺含至少两个芳环,包括对亚苯基二胺,所述稳定剂体系据说适合于使无机烃润滑油、合成烃油和聚亚烷基二醇油稳定。
美国专利号5,232,614公开了据说是有效的抗氧化剂的取代的对苯二胺,所述抗氧化剂能够保护曲轴箱润滑油在高温下长时间暴露于 氧气中之后不会增稠和形成淤渣。
WO94/22988公开了据说在发动机的运行期间改进内燃机润滑油抗磨和粘度控制性能的燃料组合物。少量所述燃料组合物在发动机运行期间与发动机润滑油结合并且这为润滑油提供了抗氧化促进。优选地,所述燃料包含至少57g/1000升不含苄基氢原子的取代的双环芳族胺如一和/或二-α-甲基苯乙烯烷基化亚苯基二胺和/或受阻酚如一苯乙烯基化一异丁烯化甲酚或二C16烷基酚。协同效应据说被芳族胺和受阻酚的混合物证实。
IN151,316公开了使用N,N′-二仲丁基-对苯二胺作为用于重型空气压缩机的溶剂萃取、脱蜡和加氢整理的矿物油基润滑油组合物的抗氧化剂。
JP53,051,206公开了N,N′-2-萘基-对苯二胺作为抗氧化剂以改进还包含二硫化物的酯或矿物油基润滑油的氧化稳定性。
JP59,020,392公开了包括N,N′-二仲丁基-对苯二胺用于油槽压力成型的润滑剂组合物。此润滑剂组合物还包含受阻酚抗氧剂。
Polish PL149,256公开了将苯基-萘基-对苯二胺用于聚亚烷基二醇基耐火液压流体。
苏联专利号1,155,615公开了包含二苯基-对亚苯基二胺用于金属冷加工的矿物油和脑磷脂基润滑剂组合物。
上述公开内容在此整体地引入作为参考。
以前,一直不认同使用与取代的对亚苯基二胺特定组合的仲二芳基胺在使润滑剂,例如润滑油,尤其是设计用于苛刻环境如其中可能发生高温和金属催化氧化反应的环境的那些润滑剂稳定方面提供出乎意料的协同效果。
发明概述
现已发现,仲二芳基胺和取代的对亚苯基二胺的组合物(任选地与取代的酚混合)在抑制润滑剂组合物的氧化方面显示协同效应,因此比仅使用所述材料中任一种更有效。所述烷基化二芳基胺与取代的对亚苯基二胺协同地发挥作用以在氧化控制方面提供显著的改进。
更具体地说,本发明涉及包含以下物质的润滑剂组合物:
(A)至少一种选自天然和合成润滑基础油的润滑油;
(B)至少一种选自由以下通式表示的仲二芳基胺的第一抗氧化剂
(R1)a-Ar1-NH-Ar2-(R2)b (I)
其中
Ar1和Ar2独立地选自芳族烃,和
R1和R2独立地选自氢和烃基,优选含6-大约100个碳原子的烃基,和
a和b独立地是0-3,条件是(a+b)不大于4;和
(C)至少一种选自具有以下通式的取代的对亚苯基二胺的第二抗氧化剂
其中R3和R4独立地选自氢和烃基,优选含1-100个碳原子的烃基;和,任选地,
(D)至少一种选自具有以下通式的取代的酚的第三抗氧化剂
其中R5、R6和R7独立地选自氢和烃基,优选含1-100个碳原子的烃基,条件是至少一个烃基在邻位且优选是具有异或叔结构的烷基。
在另一个方面,本发明涉及提高润滑剂氧化稳定性的方法,包括向所述润滑剂中添加以下物质:至少一种选自由通式(I)表示的仲二芳基胺的第一抗氧化剂,至少一种选自由通式(II)表示的取代的对亚苯基二胺的第二抗氧化剂,和任选地,至少一种选自由通式(III)表示的取代的酚的第三抗氧化剂。
具体实施方式
本文所使用的术语“烃基”包括烃基团以及大体上是烃的基团。“大体上是烃”描述此类基团,其包含不改变该基团的主要是烃性质的杂原子取代基。烃基基团的实例包括但不限于以下:
(1)烃取代基,即,脂族(例如,烷基或烯基),脂环族(例如,环烷基、环烯基)取代基,芳族取代基,芳族-、脂族-、和脂环族-取代的芳族取代基等,以及环状取代基,其中该环经由该分子的另一部份来完成(即,例如,任何两个指示取代基可以一起形成脂环族基);
(2)取代的烃取代基,即,含在本发明上下文中不改变取代基主要是烃性质的非烃基团的那些取代基;本领域技术人员将了解此类基团(例如,卤、羟基、巯基、硝基、亚硝基、硫氧基、氰基等);
(3)杂原子取代基,即,仍具有本发明上下文中的主要是烃的性质但是将包含除了碳之外的存在于另外由碳原子组成的环或链中的原子的取代基(例如,烷氧基或烷硫基)。适合的杂原子对本领域普通技术人员来说是显而易见的并且包括,例如,硫、氧、氮以及例如,吡啶基、呋喃基、噻吩基、咪唑啉基等的取代基。优选地,对于烃基基团中的每10个碳原子,将存在至多大约2个,更优选至多1个杂取代基。非常优选地,在烃基基团中将不存在此类杂原子取代基,即该烃基基团是纯烃。
如上所述,在本发明实践中用作第一抗氧化剂的仲二芳基胺可以由以下通式(I)表示:
(R1)a-Ar1-NH-Ar2-(R2)b (I)
其中Ar1和Ar2独立地选自芳族烃基,R1或R2独立地选自氢或优选含1-大约100个碳原子的烃成分或,和a和b独立地选自0-3的整数,条件是(a+b)不大于4。
第二抗氧化剂选自由通式(II)表示的取代的对亚苯基二胺:
其中R3或R4独立地选自优选含1-大约100个碳原子的烃基。
任选地,也可以存在选自由通式(III)表示的取代的酚的第三抗氧化剂:
其中R5、R6和R7独立地选自氢或优选含1-大约100个碳原子的烃基,条件是至少一个烃基在邻位并且是烷基,优选含异或叔结构的烷基。
适合于由通式(I)表示的仲二芳基胺的优选的芳基结构部分是苯基或萘基。对由通式(I)-(II)表示的仲二芳基胺和取代的对亚苯基二胺的烃基R1-R4中的碳原子类型和总数没有特殊限制,只要碳原子的总数使得润滑剂中的添加剂具有足够的热稳定性和溶解性。优选地,烃基结构部分是烷基、烯基、环烷基、环烯基、芳基、芳烷基、芳烯基、萘基和被烷基和/或烯基、羟基、羧基取代基等取代的萘基。一般而言,烃基基中碳原子的总数优选不少于6并且实际上可以多至大约100。通式(I)和(II)的一个实施方案的示例是R1-R4独立地是含1-大约100个碳原子,一个实施方案中,1-大约50个碳原子,一个实施方案中,1-大约30个碳原子的烃基,只要碳原子的总数至少是6。以下是适合于本发明实践的优选的烃基的示例:
(a)含1-大约40个碳原子的直链和支链烷基或烯基,更优选含1-20个碳原子的直链或支链烷基,例如甲基、乙基、丙基、丁基,戊基、己基、庚基、辛基、2-乙基己基,壬基、癸基、十一烷基、十二烷基,十三烷基、十四烷基、十五烷基、十六烷基、十七烷基、十八烷基、油基、十九烷基、二十烷基、上述基团的异构体和混合物等;
(b)环状烷基和烯基,例如环戊基、环己基、环庚基、环辛基、环十二烷基、环戊烯基、环己烯基、环庚烯基、环辛烯基、环十二烯基、环戊二烯基、环己二烯基、环庚二烯基、环辛二烯基等,任选地取代有一个或多个含1-40个碳原子,更优选1-16个碳原子的烷基或烯基,例如甲基、乙基、丙基、丁基、戊基、己基、庚基、辛基、壬 基、癸基、十一烷基、十二烷基、十三烷基、十四烷基、十五烷基、十六烷基、上述基团的异构体和混合物等;
(c)苯基和被一个或多个含1-40个碳原子,更优选1-16个碳原子的烷基或烯基,例如甲基、乙基、丙基、丁基,戊基、己基、庚基、辛基、壬基、癸基、十一烷基、十二烷基、十三烷基、十四烷基、十五烷基、十六烷基、上述基团的异构体等取代的苯基;
(d)萘基和被一个或多个含1-40个碳原子,更优选1-16个碳原子的烷基或烯基,例如甲基、乙基、丙基、丁基,戊基、己基、庚基、辛基、壬基、癸基、十一烷基、十二烷基、十三烷基、十四烷基、十五烷基、十六烷基、上述基团的异构体和混合物等取代的萘基;
(e)杂原子取代基,尤其是含1-40个碳原子,更优选1-20个碳原子的烷氧基烷基、烷氧基芳基,例如甲氧基甲基、乙氧基甲基、乙氧基乙基、丙氧基甲基、丙氧基乙基、丙氧基丙基等;和被一个或多个含1-16个碳原子的烷氧基如甲氧基、乙氧基、丙氧基、丁氧基、戊氧基、己氧基、庚氧基、辛氧基、壬氧基、癸氧基、十一烷氧基、十二烷氧基、十三烷基、十四烷氧基、十四烷氧基、十五烷氧基、十六烷氧基、上述基团的异构体和混合物等取代的苯基;和
(f)取代的烃取代基,尤其是羟基、羧基、硝基、氰基等。
在本发明实践中有用的由通式(I)表示的一些仲二芳基胺的实例包括二苯胺、一烷基化二苯胺、二烷基化二苯胺、三烷基化二苯胺或其混合物、3-羟基二苯胺、4-羟基二苯胺、一和/或二丁基二苯胺、一和/或二辛基二苯胺、一和/或二壬基二苯胺、苯基-α-萘胺、苯基-β-萘胺、二庚基二苯胺、一和/或二-α-甲基苯乙烯基二苯胺、一和/或二苯乙烯基二苯胺、4-(对甲苯磺酰氨基)二苯胺、4-异丙氧基二苯胺、叔辛基化N-苯基-1-萘胺、一和二烷基化叔丁基-叔辛基二苯胺的混合物。
以下是更优选的可从Crompton Corporation商购的仲二芳基胺的 示例:438、Naugalube438L、Naugalube640、Naugalube635、Naugalube680、Naugalube AMS、Naugalube APAN和Naugard PANA。
在本发明实践中有用的由通式(II)表示的一些取代的对亚苯基二胺的实例包括:N,N′-二异丙基-对苯二胺、N,N′-二仲丁基-对苯二胺、N,N′-双(1,4-二甲基戊基)-对苯二胺、N,N′-双(1-乙基-3-甲基戊基)-对苯二胺、N,N′-双(1-甲基庚基)-对苯二胺、N,N′-二环己基-对苯二胺、N,N′-二苯对苯二胺、N,N′-二(萘基-2)-对苯二胺、N-异丙基-N′-苯基-对苯二胺、N-(1,3-二甲基丁基)-N′-苯基-对苯二胺、N-(1-甲基庚基)-N′-苯基-对苯二胺、N-环己基-N′-苯基-对苯二胺。
以下是优选的可从Flexsys Corporation商购的取代的对亚苯基二胺的示例:IPPD、Santoflex6PPD、Santoflex44PD、Santoflex77PD、Santoflex134PD、Santoflex1350PD、Santoflex715PD和Santoflex434PD。
以下是更优选的可从Crompton Corporation商购的取代的对亚苯基二胺的示例:4L、Flexzone6H、Flexzone7L、Flexzone11L、Flexzone12L、Flexzone15L、Naugalube403、Naugalube410和Naugalube420。
随着所述烃基结构部分的组成的广泛变化,任选的在本发明实践中有用的由通式(III)表示的取代的酚抗氧剂可以包括烷基化一苯酚、烷基化氢醌、羟基化硫代二苯醚、烷叉基双酚;酰胺基苯酚;和受阻酚取代的链烷酸的酯和酰胺。
以下是此类酚抗氧剂的实例:2,6-二叔丁基-4-甲基苯酚、2,6-二叔丁基苯酚、2-叔丁基-4,6-二甲基苯酚、2,6-二叔丁基-4-乙基苯酚、2,6-二叔丁基-4-异丁基苯酚、2,6-双(α-甲基苄基)-4-甲基苯酚、2-α-甲基苄基-4-甲基苯酚、2,4,6-三环己基苯酚、2,6-二叔丁基-4-甲氧基甲基苯酚等;2,5-二叔丁基-氢醌、2,5-二叔戊基-氢醌等;2,2′-硫代双(6-叔丁基-4-甲基苯酚)、2,2′-硫代双(4-辛基苯酚)、4,4′-硫代双(6-叔丁基-3-甲基苯酚)、4,4′-硫代双(6-叔丁基-2- 甲基苯酚)等;2,2′-亚甲基双(6-叔丁基-4-甲基苯酚)、2,2′-亚甲基双[4-甲基-6-(α-甲基环己基)苯酚]、2,2′-亚甲基双(4-甲基-6-环己基苯酚)、2,2′-亚甲基双(4,6-二叔丁基苯酚)、4,4′-亚甲基双(2,6-二叔丁基苯酚)、1,1-双(5-叔丁基-4-羟基-2-甲基苯基)丁烷、二(3-叔丁基-4-羟基-5-甲基苯基)双环戊二烯、甘醇双[3,3-双(3′-叔丁基-4′-羟苯基)丁酸酯]等;1,3,5-三(3,5-二叔丁基-4-羟苄基)-2,4,6-三甲基苯、二(3,5-二叔丁基-4-羟苄基)硫醚、3,5-二叔丁基-4-羟苄基巯基乙酸异辛基酯、3,5-二叔丁基-4-羟苄基膦酸二(十八烷基)酯、1,3,5-三(3,5-二叔丁基-4-羟苄基)-异氰脲酸酯、1,3,5-三(4-叔丁基-3-羟基-2,6-二甲基苄基)-异氰脲酸酯、双(4-叔丁基-3-羟基-2,6-二甲基苄基)二硫代对苯二甲酸酯、3,5-二叔丁基-4-羟苄基膦酸一乙基酯钙盐等;4-羟基月桂酸酰替苯胺、4-羟基硬脂酸酰替苯胺、2,4-双辛基巯基-6-(3,5-二叔丁基-4-羟基苯胺)-s-三嗪、N-(3,5-二叔丁基-4-羟苯基)氨基甲酸辛基酯等;和用甲醇、辛醇、十八醇、1,6-己烷二醇、新戊二醇、硫代二甘醇、二甘醇、三甘醇或季戊四醇等酯化的3,5-二叔丁基-4-羟基苯-3-丙酸。
以下是可从Ciba Corporation商购的适合用于本发明实践的酚抗氧剂的示例:IrganoxL101、IrganoxL107、IrganoxL109、IrganoxL115、IrganoxL118和IrganoxE201;和可从Crompton Corporation商购的:BHT、Naugard SP、Naugard529、Naugard76、Antioxidant431和Nauga lube531。
在本发明润滑油组合物的制备中,可以按各自大约0.01-大约10wt%,优选大约0.1-大约5wt%的量将组分(B),选自具有上述通式(I)的仲二芳基胺,和组分(C),具有上述通式(II)的取代的对亚苯基二胺在所述组合物中共混。也可以按大约0.01-大约10总wt%,优选大约0.1-大约5wt%的量将任选的组分(D),选自具有通式(III)的取代的酚在润滑油组合物中共混。本发明润滑油组合物中采用的仲二芳基胺与取代的对亚苯基二胺的含量比可以实际上按所有比例。但是优选地,该比例将为1:99-99:1重量份,更优选,90:10-10:90重 量份。如果包括任选的取代的酚,三种抗氧化剂的含量比例可以实际上按所有比例,只要仲二芳基胺与取代的对亚苯基二胺的含量比为1:99-99:1重量份,更优选,90:10-10:90重量份。
可以根据刚才限定的含量比例将本发明的组分预混合,然后添加到(或者可以单独地添加到)润滑剂中,根据需要,通过温和加热(50℃)和机械搅拌进行添加。
本发明的抗氧化剂混合物可以与润滑油中常用的其它添加剂,以及其它抗氧化剂结合使用。常用于润滑油的添加剂是,例如,分散剂、洗涤剂、抗磨剂、抗氧化剂、摩擦改进剂、密封溶胀剂、破乳化剂、VI(粘度指数)改进剂、倾点下降剂、消泡剂、防腐剂和金属钝化剂。这些添加剂是本领域技术人员熟知的并且对用于本发明的这些添加剂的类型没有特殊的限制。美国专利号5,498,809公开了有用的润滑油组合物添加剂,其公开内容在此整体引入作为参考。
分散剂的实例包括聚异丁烯琥珀酰亚胺、聚异丁烯琥珀酸酯、Mannich碱无灰分散剂等。洗涤剂的实例包括金属和无灰的烷基酚盐、金属和无灰的硫化烷基酚盐、金属和无灰的烷基磺酸盐、金属和无灰的烷基水杨酸盐、金属和无灰的水杨醇衍生物等。
可以与本发明的抗氧化剂混合物结合使用的抗氧化剂的实例包括二甲基喹啉、三甲基二氢喹啉和衍生自它们的低聚物组合物、硫代丙酸盐、金属二硫代氨基甲酸盐、油溶性铜化合物等。可与本发明添加剂结合使用的抗磨损添加剂的实例包括有机硼酸盐、有机亚磷酸盐、有机磷酸盐、有机含硫化合物、硫化烯烃、硫化脂肪酸衍生物(酯)、氯化石蜡、二烷基二硫代磷酸锌、二芳基二硫代磷酸锌、二烷基二硫代磷酸酯、二芳基二硫代磷酸酯、磷硫化烃等。以下物质是此类添加剂的示例并且可从Lubrizol Corporation商购:Lubrizol677A、Lubrizol1095、Lubrizol1097、Lubrizol1360、Lubrizol1395、Lubrizol5139和Lubrizol5604等;从Ciba Corporation商购的 62、Irgalube211、Irgalube232、Irgalube349、Irgalube353、Irgalube TPPT、OPH,等;和从Crompton Corporation 商购的:600、Weston DLP、Weston TPP等。
摩擦改进剂的实例包括脂肪酸酯和酰胺、有机钼化合物、二烷基二硫代氨基甲酸钼、二烷基二硫代磷酸钼、二硫化钼、二烷基二硫代氨基甲酸三钼簇合物、无硫钼化合物等。以下物质是钼添加剂的示例并且可从R.T.Vanderbilt Company,Inc.商购:Molyvan A、MolyvanL、Molyvan807、Molyvan856B、Molyvan822、Molyvan855等。以下物质也是此类添加剂的示例并且可从Asahi Denka Kogyo K.K.商购:SAKURA-LUBE100、SAKURA-LUBE165、SAKURA-LUBE300、SAKURA-LUBE310G、SAKURA-LUBE321、SAKURA-LUBE474、SAKURA-LUBE600、SAKURA-LUBE700等。以下物质也是此类添加剂的示例并且可从AkzoNobel Chemicals GmbH商购:Ketjen-Ox77M、Ketjen-Ox77TS等。Naugalube MoIyFM也是此类添加剂的示例并且可从CromptonCorporation商购。
VI改进剂的实例包括烯烃共聚物和分散剂烯烃共聚物等。倾点下降剂的实例是聚甲基丙烯酸酯等。消泡剂的实例是聚硅氧烷等。防锈剂的实例是聚氧化烯多元醇、苯并***衍生物等。金属钝化剂的实例包括***、苯并***、2-巯基苯并噻唑、2,5-二巯基噻二唑、甲苯基***衍生物、N,N′-二亚水杨基-1,2-二氨基丙烷等。以下是金属钝化剂的示例并且可从Ciba Corporation商购:30、Irgamet39和Irgamet42。
润滑剂组合物
当组合物包含这些添加剂时,通常以满足以下条件的量将它们混入基础油中,即其中的添加剂有效提供它们正常所附的作用。此类添加剂的代表性的有效量在表1中示出。
当使用其它添加剂时,虽然不是必要的,但是可能希望制备添加剂浓缩物,该添加剂浓缩物包含本发明主题添加剂的浓缩溶液或分散体(以上文的浓的量),以及一种或多种所述其它添加剂(当构成添加剂混合物时,所述浓缩物在此称作复合添加剂),这样可以将数种添加剂同时添加到基础油中以形成润滑油组合物。所述添加剂浓缩物进入润滑油的溶解可以通过溶剂来促进和通过在温和加热下的混合来促进,但是这不是必要的。所述浓缩物或复合添加剂将通常经配制以适当的量包含添加剂,该适当的量满足当将所述复合添加剂与预定量的基础润滑剂结合时提供最终制剂中的所需浓度。因此,可以将本发明的主题添加剂与其它合乎需要的添加剂一起添加到少量基础油或其它相容性溶剂中以形成复合添加剂,该复合添加剂通常以占合适比例存在的添加剂的大约2.5-大约90wt%,优选大约15-大约75wt%,更优选大约25wt%-大约60wt%的总量包含活性成分,剩余部分是基础油。最 终制剂通常可以使用大约1-20wt%复合添加剂,剩余部分是基础油。
在此表示的所有重量百分数(除非另有说明)基于添加剂的活性成分(AI)含量,和/或基于任何复合添加剂,或制剂的总重量,该总重量将是每种添加剂的AI重量加上全部油或稀释剂的重量的总和。
一般而言,本发明的添加剂在各种润滑油基础原料中是有用的。所述润滑油基础原料是在100℃下运动粘度为大约2-大约200cSt,更优选大约3-大约150cSt,非常优选大约3-大约100cSt的任何天然或合成润滑油基础原料级分。
所述润滑油基本原料可以衍生自天然润滑油、合成润滑油或它们的混合物。适合的润滑油基础原料包括通过将合成蜡和蜡异构化获得的基础原料,以及通过将原油的芳族和极性组分加氢裂解(而不是溶剂萃取)制备的加氢裂化基础原料。天然润滑油包括:动物油,例如猪油,牛油,植物油(例如,低芥酸菜籽油、蓖麻油、向日葵油),石油,矿物油和衍生自煤炭或页岩的油。
合成油包括烃油和卤取代的烃油,如聚合和互聚合烯烃、通过费托技术制备的气体液化油、烷基苯,聚苯、烷基化二苯醚、烷基化苯硫醚以及它们的衍生物、类似物、同系物等。合成润滑油还包括氧化烯聚合物、互聚物、共聚物和它们的衍生物,其中末端羟基基团已被酯化、醚化等改性。
另一类适合的合成润滑油包含二羧酸与各种醇的酯。作为合成油有用的酯还包括由C5-C18单羧酸和多元醇和多元醇醚制备的那些。作为合成油有用的其它酯包括由α-烯烃和用短或中等链长的醇酯化的二羧酸的共聚物制成的那些。
硅基油,例如聚烷基-、聚芳基-、聚烷氧基-、或聚芳氧基-硅氧烷油和硅酸盐油,是另一类有用的合成润滑油。其它合成润滑油包括含磷的酸的液体酯、聚合物四氢呋喃、聚α-烯烃等。
该润滑油可以衍生自未精炼的、精炼的、再精炼的油、或者其混合物。未精炼的油直接由天然源物质或者合成源物质(例如,煤炭、页岩、或焦油和沥青)获得,而没有进一步的纯化或处理。未精炼的 油的实例包括由蒸馏操作直接获得的页岩油、由蒸馏直接获得的石油、或由酯化方法直接获得的酯油,然后在没有进一步处理的情况下使用它们中的每一种。精炼油与未精炼油相似,不同在于精炼油已经在一个或多个纯化步骤中得到处理以改进一种或多种性能。适合的纯化技术包括蒸馏、加氢处理、脱蜡、溶剂萃取、酸或碱萃取、过滤、渗滤等,所有这些是为本领域技术人员所熟知的。再精炼油是通过与用来获得精炼油相似的方法处理精炼油来获得的。这些再精炼油亦称回收或再加工油,并经常通过用于除去废添加剂和油分解产物的技术进行另外的处理。
衍生自蜡的加氢异构化的润滑油基础原料也可以单独地或与上述天然和/或合成基础原料结合起来使用。此种蜡的异构化物油通过在加氢异构化催化剂上将天然或合成蜡或其混合物加氢异构化而制备。天然蜡通常是通过矿物油的溶剂脱蜡回收的松弛蜡;合成蜡通常是通过费-托法制备的蜡。所得的异构产物通常经受溶剂脱蜡和分馏法处理以回收具有特定粘度范围的各种馏分。蜡异构化物还以具有非常高的粘度指数(通常具有至少130,优选至少135或更高的VI)和在脱蜡之后具有大约-20℃或更低的倾点为特征。
用于本发明实践的润滑油可以选自如American PetroleumInstitute(API)Base Oil Interchangeability Guidelines中广泛规定的I-V组中的任何基础油。该五组基础油在表2中进行了描述。
表2
API基础油分类 硫(%) 饱和物(%) 粘度指数 |
组I >0.03 和/或 <90 80-120 |
组II ≤0.03 和 ≥90 80-120 |
组III ≤0.03 和 ≥90 ≥120 |
组IV 所有聚α-烯烃(PAO) |
组V 没有包括在组I、II、III或IV中的所有其它 |
本发明添加剂在许多不同润滑油组合物中作为组分是尤其有用的。可以将添加剂加入各种具有润滑粘度的油中,包括天然和合成润滑油以及它们的混合物。可以将该添加剂放入用于火花点火和压缩点火的内燃机的曲轴箱润滑油。该组合物还可以用于燃气发动机润滑剂、蒸汽-燃气轮机润滑剂、自动传动流体、齿轮润滑剂、压缩机润滑剂、金属加工润滑剂、液压流体、和其它润滑油和润滑脂组合物。所述添加剂也可以用来使发动机燃料组合物稳定。
本发明的优点和重要特征将在以下实施例中说明。
实施例
根据本发明实践结合使用对亚苯基二胺和仲二芳基胺的协同效应已经在发动机油制剂中通过以下两个加速氧化试验得到了证实:加压差示扫描量热法(PDSC)、和中-高温热氧化发动机油模拟试验(TEOST)MHT。
用于所述试验的发动机油制剂包含可商购的以下组分。对本发明上下文中材料的类型和精确组成没有特殊限制。
组成 | 用量,wt% |
基础油,第II组 | 85 |
高碱性磺酸盐洗涤剂 | 2.5 |
抗磨/EP剂 | 1.0 |
琥珀酰亚胺分散剂 | 6.5 |
VI改进剂 | 5.0 |
加压差示扫描量热法结果
加压差示扫描量热法(PDSC)测量表4中的每种共混物的氧化感应时间(OIT)。所用PDSC仪器是由Mettler-Toledo,Inc(Switzerland)制造的Mettler DSC27HP。PDSC方法在每个轮次过程中在恒定氧气压力下使用钢槽。该仪器具有典型的±2.5分钟的重复率,于100分钟的OIT内具有95%的置信度。PDSC试验条件在表3中给出。在一个PDSC轮次开始时,用氧气将钢槽加压并以40℃/分钟的速率加热到规定的等温温度。从样品达到其等温温度的时间测量感应时间直到观察到热 函变化。氧化感应时间越长,油的氧化稳定性越好。
表3.PDSC试验条件
测验参数 | 设定 |
等温温度 | 200℃ |
O2气压力 | 500psi |
通过槽的O2气流速率 | 100ml/min |
催化剂 | 50ppm铁 |
样品容器 | 开口铝盘 |
样品大小 | 1.0-2.0mg |
感应时间 | 热函变化 |
试验中使用的仲二芳基胺主要是一,二和三壬基二苯基胺的复杂混合物并且目前以商品名Naugalube438L销售,而试验中使用的取代的对亚苯基二胺是目前以商品名Naugalube420销售的N-(己基/庚基)-N′-苯基-对亚苯基二胺的共混物,它们都可从CromptonCorporation商购。根据本发明的实践所添加的包括仲二芳基胺和取代的对亚苯基二胺的抗氧化剂的总量在每种共混物中为1.5wt%。将所有试验共混物在氮气气氛下机械混合15分钟。对于每50克制备的试验共混物,在PDSC测试之前,添加40μL油溶性环烷酸铁(6wt%,在矿物油中)以促成在油中有50ppm铁。在表3描述的PDSC条件下在200℃测试每种共混物两次。每个重复轮次的平均和标准偏差在表4中给出。在数据表中的共混物3、4和5的OIT结果证实包含根据本发明的抗氧化剂混合物的合适混合物的润滑油组合物具有优异的氧化稳定性。
表4PDSC结果
热氧化发动机油模拟试验(TEOST)MHT
仲二芳基胺和取代的对亚苯基二胺的混合物在使发动机油制剂稳定方面的协同效应已经通过中-高温热氧化发动机油模拟试验(TEOST)MHT更清楚地得到证实,所述试验测定通过在热氧化和催化条件下让8.5试验油连续地重复通过而在特制钢杆上形成的沉积物。所使用的仪器由Tannas Co.制造并具有0.15(x+16)mg的典型重复性,其中x是两个或更多个重复试验结果的平均值。TEOST试验条件在表5中列出。获得的沉积物的量越少,油的氧化稳定性越好。
试验中使用的仲二芳基胺目前以商品名Naugalube438L销售的主要是一,二和三壬基二苯基胺的复杂混合物,而试验中使用的取代的对亚苯基二胺是目前以商品名Naugalube420销售的N-(己基/庚基)-N′-苯基-对亚苯基二胺的共混物,它们都可从Crompton Corporation商购。根据本发明的实践所添加的包括仲二芳基胺和取代的对亚苯基二胺的抗氧化剂的总量在每种共混物中为1.5wt%。如表6中的数据所示,对于共混物8、9和10来说,获得的显著更少的沉积物量证实包含本发明抗氧化剂共混物的合适混合物的润滑油组合物具有优异的氧化稳定性而在TEOST中产生更少量的沉积物。
表5TEOST MHT试验条件
试验参数 | 设定 |
试验时间 | 24小时 |
杆温度 | 285℃ |
样品大小 | 8.5g(8.4g油和0.1g催化剂的混合物) |
样品流速 | 0.25g/min |
流速(干空气) | 10mL/min |
催化剂 | 含Fe、Pb和Sn的油溶性混合物 |
表6.TEOST结果
考虑到在不脱离基于本发明的原理的情况下可以作出的许多改变和修改,应该参照所附权利要求书来理解本发明提供的保护范围。
Claims (4)
1.润滑剂组合物,包含:
(A)至少一种选自天然和合成润滑基础油的润滑油;
(B)商品名为Naugalube 438L的占所述组合物总重量0.1~5重量%的一、二和三壬基二苯基胺的混合物;和
(C)商品名为Naugalube 420的占所述组合物总重量0.1~5重量%的N-(己基/庚基)-N′-苯基-对亚苯基二胺的共混物。
2.权利要求1的组合物,还包含至少一种附加的选自分散剂、清净剂、防锈剂、抗氧化剂、金属钝化剂、抗磨剂、消泡剂、摩擦改进剂、密封溶胀剂、破乳化剂、粘度指数改进剂和倾点下降剂的添加剂。
3.提高润滑剂组合物的氧化稳定性的方法,包括向所述润滑剂中添加以下物质:
(A)商品名为Naugalube 438L的占所述组合物总重量0.1~5重量%的一、二和三壬基二苯基胺的混合物;和
(B)商品名为Naugalube 420的占所述组合物总重量0.1~5重量%的N-(己基/庚基)-N′-苯基-对亚苯基二胺的共混物。
4.权利要求3的方法,其中该组合物还包含至少一种附加的选自分散剂、清净剂、防锈剂、抗氧化剂、金属钝化剂、抗磨剂、消泡剂、摩擦改进剂、密封溶胀剂、破乳化剂、粘度指数改进剂和倾点下降剂的添加剂。
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US11/145,493 US7704931B2 (en) | 2004-12-10 | 2005-06-03 | Lubricant compositions stabilized with multiple antioxidants |
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EP1833952B1 (en) | 2015-12-23 |
CN102816626A (zh) | 2012-12-12 |
WO2006065344A1 (en) | 2006-06-22 |
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