CN1071685A - 油料和燃料油组合物 - Google Patents

油料和燃料油组合物 Download PDF

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CN1071685A
CN1071685A CN92111644A CN92111644A CN1071685A CN 1071685 A CN1071685 A CN 1071685A CN 92111644 A CN92111644 A CN 92111644A CN 92111644 A CN92111644 A CN 92111644A CN 1071685 A CN1071685 A CN 1071685A
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oil
alkyl
composition
fuel
ester
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CN1038254C (zh
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K·卢塔思
J·D·布兰德
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ExxonMobil Chemical Patents Inc
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Exxon Chemical Patents Inc
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Abstract

通过添加含下列重复结构单元的聚合物和含芳 基的梳型聚合物的添加剂组合物可改进油料和燃料 油组合物的各种性质。

Description

本发明涉及各种添加剂组合物及其在改进油料和燃料油组合物性质方面的应用。
业已知道，在低温下蜡会从油料和燃料油中分离出来，因而使某些性质受到损害。还已知道，使用添加剂可改进这些性质，如改进低温流动性以及防止在放置过程中蜡在重力的作用下的沉降。前一种添加剂有时称为低温流动改进剂，而后一种添加剂有时称为抗蜡沉降添加剂。
描述这样的添加剂及其应用的专利说明书的例子是US    3048479、3961916、3252771、2542542、3444082、4211534、4375973和4402708，GP    1263152、1469016、1468588、2129012、2923645和1209676，JP    5654038、5654037和5540640。
EP-A-0225688描述了衣康酸酯和柠康酸酯聚合物和共聚物用于改进油料（原油或润滑油）和燃料油（如残渣燃料油、中间馏分油燃料和喷气燃料）的低温流动性，或作为润滑油脱蜡助剂，可使聚合物和共聚物适合所涉及的特定油料或燃料油。该专利描述了数均分子量（用凝胶渗透色谱测定）为1000～500000.的聚合物和共聚物。并例举了分子量为20000或20000以上的聚合物和共聚物。
在油料和燃料油中使用EP-A-0255688范围内的聚合物带来的问题是，它们可能使流动改进添加剂的低温流动性能变差。本发明通过使用某些组合的梳型聚合物可克服这一缺点，它们将在下文描述，並在实施例中说明。
国际专利申请号PCT/GB91/00622（公布号WO91/16407）描述了使用EP-A-0255688范围内的数均分子量为1000～20000的聚合物如与其他添加剂一起作为馏分油燃料的低温流动改进剂，其中梳型聚合物已提到，但未具体举例说明。
第一方面，本发明提供一种下列组分的添加剂组合物：
（ⅰ）一种含下列结构单元的聚合物
Figure 921116446_IMG5
其中，X为一整数，Y为0或一整数。在该聚合物中X和Y的总和至少为2。结构单元（Ⅱ）与（Ⅰ）的比为0～2，结构单元（Ⅱ）与（Ⅲ）的比为0～2，其中，
R1和R2是相同的或不同的，都为C10～C30烷基，
R3代表H、-OOCR6、C1～C30烷基、-COOR6、-OR6和芳基或烷芳基或卤素。
R4代表H或甲基。
R5代表E、C1～C30烷基、或-COOR6，
R6代表C1～C22烷基，
R1、R2、R3、R4、R5和R6中任何一个都可以被惰性取代，
（ⅱ）一种在聚合物主链上有芳基和烃基的梳型聚合物，其中烃基有10个或10个以上碳原子。组分（ⅱ）最好是有下列通式的聚合物：
Figure 921116446_IMG6
其中，D为R7、C（O）.OR、OC（O）.R7、R8C（O）.OR7、或OR7，
E为H或CH3或D或R8。
G为H或D。
m为1.0（均聚物）～0.4（摩尔比）
J为H、R8、芳基或杂环基、R8CO.OR7.
K为H、C（O）.OR8，OC（O）.R8，OR8，C（O）OH.
L为H、R8、C（O）.OR8、OC（O）.R8、芳基、C（O）OH.
n为0～0.6（摩尔比）
R7为含10个或10个以上碳原子的烃基.
R8为C1或更高的烃基，只要J和L至少一个是芳基。
最好R7有10～30个碳原子和R8有1～30个碳原子。
第二方面，本发明提供作为原油、润滑油或燃料油的流动改进剂或润滑油脱蜡助剂的本发明第一方面的添加剂组合物的应用。
第三方面，本发明提供一种含大量原油、润滑油或燃料油和少量本发明第一方面的添加剂组合物的原油、润滑油或燃料油组合物。
第四方面，本发明提供一种含有分散在与原油、润滑油或燃料油相容的液体介质中的本发明第一方面的添加剂组合物的混合物的添加剂浓缩物。
第五方面，本发明提供一种改进原油、润滑油或燃料油的流动性质或帮助润滑油脱蜡的方法，其中包括把本发明第一方面的添加剂组合物加到油料中。
现在将更详细地描述本发明的各个特点。
组分（ⅰ）
聚合物（ⅰ）可能是一种二烷基衣康酸酯或二烷基柠康酸酯的均聚物或一种二烷基衣康酸酯或二烷基柠康酸酯与脂族烯烃、乙烯基醚、链烷酸的乙烯基酯、不饱和酸的烷基酯、芳族烯烃、乙烯基卤化物或二烷基富马酸酯或马来酸酯的共聚物;或者聚合物（ⅰ）可能是一种二烷基衣康酸酯或二烷基柠康酸酯与脂族烯烃、C2～C30链烷酸的乙烯基酯或烷基取代的乙烯基酯的共聚物。
R1和R2最好都是直链基，虽然它们也可以是支链的。如果是支链的，支链最好在1或2位是单甲基。R1和R2的例子是癸基、十二烷基、十六烷基和二十烷基。R1和R2中的每一个都可是单一的C10～C30烷基或混合烷基。R1和R2都是C12～C20混合烷基的聚合物特别适用作中间馏分油燃料油的流动改进剂。R1和R2都是C16～C22烷基的聚合物特别适用于重质燃料油和原油，而R1和R2都是C10～C18烷基的聚合物特别适用于润滑油。这样的特别有用的聚合物可为均聚物或共聚物。
当作为共聚单体时，二烷基衣康酸酯或二烷基柠康酸酯有下列通式：
Figure 921116446_IMG7
其中，R3、R4和R5如上面所规定的。这样的共聚单体可为混合物。
当这样的共聚单体是脂族烯烃时，R3和R5代表H或C1～C30烷基，最好是正构烷基，它们是相同的或不同的。如当R3、R4和R5都是H时，烯烃是乙烯，而当R3是甲基，R4和R5是H时，烯烃是丙烯。当R3是烷基，R4和R5最好是H。其他适合的烯烃的例子是1-丁烯、2-丁烯、异丁烯、1-戊烯、1-己烯、1-十四烯、1-十六烯和1-十八烯及其混合物。
其他这样的共聚单体是C2～C31链烷酸的乙烯基酯或烷基取代的乙烯基酯：在乙烯基酯中，当R3为R6COO-时，R4为H和R5为H;在烷基取代的乙烯基酯中，当R3为R6COO-时，R4为甲基和/或R5为C1～C30烷基。未取代的乙烯基酯更适合，其例子是醋酸乙烯酯、丙酸乙烯酯、丁酸乙烯酯、癸酸乙烯酯、十六烷酸乙烯酯和硬脂酸乙烯酯。
另一类共聚单体是不饱和酸的烷基酯，如当R3为R6OOC-时，R5为H或C1～C30烷基。当R4和R5为H时，共聚单体是丙烯酸烷基酯。当R4为甲基时，共聚单体是甲基丙烯酸酯或C1～C30烷基取代的甲基丙烯酸酯。丙烯酸的烷基酯的例子是丙烯酸甲酯、丙烯酸正己酯、丙烯酸正癸酯、丙烯酸正十六烷基酯、丙烯酸正十八烷基酯和丙烯酸2-甲基十六烷基酯。甲基丙烯酸烷基酯的例子是甲基丙烯酸丙酯、甲基丙烯酸正丁酯、甲基丙烯酸正辛酯、甲基丙烯酸正十四烷基酯、甲基丙烯酸正十六烷基酯和甲基丙烯酸正十八烷基酯。其他例子是相应的酯。其中R5为烷基，如甲基、乙基、正己基、正癸基、正十四烷基和正十六烷基。
另一类共聚单体是，当R3和R5是R6OOC-，如当它们是C1～C22二烷基富马酸酯或马来酸酯时，烷基可能是正构烷基或支链烷基，如正辛基、正癸基、正十四烷基、正十六烷基或正十八烷基。
共聚单体的其他例子是R3为芳基的共聚单体。当R4和R5是H，和R3是苯基时，共聚单体是苯乙烯，当R4和R5中的一个是甲基时，共聚单体是甲基苯乙烯，例如α-甲基苯乙烯。当R3为芳基时，另一例子为乙烯基萘。当R3为烷芳基时，另一些例子例如是取代的苯乙烯、如乙烯基甲苯或4-甲基苯乙烯。
当R3是卤素（如氯）时，另一共聚单体是乙烯基氯化物（即R4和R5为氢）。
正如所述，一些或全部R1、R2、R3、R4、R5和R6基可被惰性取代;例子是被一个或多个卤素原子（如氯或氟）取代。例如，共聚单体可为三氯醋酸乙烯酯。另一方面，惰性取代基可为烷基，如甲基。
当结构单元（Ⅱ）与（Ⅰ）的比和结构单元（Ⅱ）与（Ⅲ）的比是0时，聚合物是衣康酸酯或柠康酸酯的均聚物，当比值为2时，聚合物为共聚物。该比值最好为0.5～1.5。通常，共聚物只由结构单元（Ⅰ）和（Ⅱ）组成，或仅由结构单元（Ⅱ）和（Ⅲ）组成，但也不排除其他结构单元。但是，在共聚物中结构单元（Ⅰ）和（Ⅱ）或（Ⅱ）和（Ⅲ）的重量百分数希望至少为60%，最好为至少70%。
组分（ⅰ）聚合物的分子量无论均聚物或共聚物都为1000～500000，可取的是1000～20000，更可取的是1000～10000，最可取的是2200～5000，分子量用凝胶渗透色谱（GPC）相对于聚苯乙烯标准物测定，为数均分子量。
均聚物和共聚物一般通过单体单独聚合或在烃类溶剂（如庚烷、苯、环己烷或白油）中聚合制备，温度一般为20～150℃，通常用氢过氧化物或偶氮型催化剂（如苯甲酰氢过氧化物或偶氮二异丁腈在一层惰性气体（如N2或CO2）下催化，以便隔绝氧。聚合物在压力下在高压釜中或在回流情况下制备。
为了制备共聚物，聚合反应混合物每摩尔二烷基衣康酸酯或二烷基柠康酸酯可含高达2摩尔共聚单体（如醋酸乙烯酯）。
在本发明的实践中，可使用一种以上组分（ⅰ）。
例如，组分（ⅰ）与组分（ⅱ）的比可为10∶1～1∶10重量比。
组分（ⅱ）
梳型聚合物在结构上在直链聚合物和支链聚合物之间，在聚合物主链（如聚亚甲基主链）有长的脂族烃侧链，主链可被间断或不被间断。它们例如在“Conb-ljke    Polymers，Structure    and    Properties”中描述，由N.A.Plate和V.P.Shibaev著，载于J.Polymer    Science：Macromolecular    Reviews，第8卷117-253页（1974），John    Wiley和Son出版。
“烃基”指的是含氢和碳的基团，如脂族基团，它可被一个或多个不足以改变基团的烃基性质的杂原子（如O、N、S）间断。
聚合物最好具有下列通式：
Figure 921116446_IMG8
其中，D、E、K、m和n如上面所规定的，J是芳基，可被取代或未取代。
更具体地说，组分（ⅱ）最好是单体（a）和（b）的共聚物，其中
（a）是一种酯，是单烷基或二烷基的富马酸酯、马来酸酯、衣康酸酯、柠康酸酯、中康酸酯、反戊烯二酸酯或顺戊烯二酸酯，其中烷基有8～23个碳原子。
（b）是一种每分子有8～40个碳原子的芳族取代的烯烃，如Ar-CH＝CH2，其中Ar为芳族取代基。
（a）最好是二烷基酯，例如富马酸酯，但单烷基酯也是适用的，如富马酸酯。烷基最好是直链烷基，虽然如果希望的话，也可使用支链烷基。适合的烷基的例子是癸基、十二烷基、十四烷基、十六烷基、十八烷基、二十烷基、二十二烷基或其混合物。烷基最好含10～18个碳原子，如10～14个碳原子。其中酯为二烷基酯，如二烷基富马酸酯，两个烷基可不同。
在（b）中。芳族取代基最好是苯基取代基，特别可取的单体是苯乙烯和α和β烷基苯乙烯（如α-甲基苯乙烯和β-甲基苯乙烯），它们可在苯环上被取代，例如用一个或多个烷基或卤素原子取代。这样的烷基取代基例如可有1～20个碳原子。
（b）对（a）的摩尔比例如为1∶1.5～1.5∶1，最好是1∶1.2～1.2∶1，如1∶1。（a）和（b）的共聚物的分子量可为2000～100000，最好为5000～50000，用凝胶渗透色谱（GPC）相对于聚苯乙烯标准测定。
组分（ⅱ）可取的例子是苯乙烯-马来酸酯共聚物或苯乙烯-富马酸酯共聚物，在本发明中它们最好与数均分子量为1000～20000的聚衣康酸酯（作为组分（ⅰ））一起使用。
在本发明的实践中，可使用一种以上组分（ⅱ）。
其他低温流动改进剂
本发明的添加剂组合物可与一种或多种其他低温流动改进剂（作共添加剂）一起使用，如本专业已知的那些低温流动改进剂。例子是与由组分（ⅰ）或组分（ⅱ）组成的聚合物不同的梳型聚合物;聚亚氧烷基酯醚、醚、酯/醚、酰胺/酯及其混合物;乙烯不饱和酯共聚物;极性化合物（离子型或非离子型，如EP-A-0225688中描述的）;羰基硫化合物和烃类聚合物
现将其他低温流动改进剂进一步详细地描述如下：
梳型聚合物
例子是有下列通式的那些梳型聚合物
其中，D为R、CO.OR、OCO.R、R1CO.OR或OR，
E为H或CH3或D或R1，
G为H或D，
m为1.0（均聚物）～0.4（摩尔比），
J为H、R1、芳基或杂环基，或R1CO.OR，
K为H、CO.OR1、OCO.R1、OR1或CO2H，
L为H、R1、CO.OR1、OCO.R1、芳基或CO2H，
n为0.0～0.6（摩尔比），
R≥C10，
R1≥C1。
如果需要的话，另一单体可三聚。
适宜的梳型聚合物的例子是富马酸酯/醋酸乙烯酯共聚物，特别是EP0153176和0153177中描述的那些;酯化的烯烃/马来酐共聚物;α-烯烃/马来酸酐共聚物的聚合物和共聚物;α-烯烃的聚合物和共聚物;苯乙烯和马来酸酐的酯化共聚物;衣康酸或柠康酸的烷基酯的聚合物，如其中烷基有16～18个碳原子和聚合物的数均分子量为1000～20000。
聚氧化烯化合物
例子是聚氧化烯基酯、醚、酯/醚以及它们的混合物，特别是那些含有至少一个，最好两个C10～C30直链饱和烷基和一个聚亚氧烷基二醇基，分子量一直到5000。最好是200～5000，在所述的聚亚氧烷基二醇的烷基含1～4个碳原子。这些物质构成EP0061895A2的内容，另一些这样的添加剂在US 4491455中描述。
可使用的优选的酯、醚或酯/醚在结构上可用下列通式描述
R-O（A）-O-R2
其中，R和R2是相同的或不同的，可能是
（a）正构烷基
（b）正构烷基
Figure 921116446_IMG10
Figure 921116446_IMG11
例如，n为1～30，烷基是直链饱和烷基，含有10～30个碳原子，A代表二元醇的聚亚烷基段，其中亚烷基有1～4个碳原子，如聚氧化亚甲基、聚氧乙烯或聚氧三亚甲基部分，它基本上是直链的;带低碳烷基侧链的某种分支度（如在聚亚氧丙二醇）是允许的，但二元醇应基本上是直链的。A也可含氮。
适宜的二元醇一般是基本上直链聚乙二醇（PEG）和聚丙二醇（PPG），分子量大约为100～5000，最好是200～2000。酯是优选的，含有10～30个碳原子的脂肪酸用于与二元醇反应生成酯添加剂，优选使用C18～C24脂肪酸，特别是二十二烷酸。酯也可通过聚乙氧化脂肪酸或聚乙氧化醇的酯化来制备。
聚氧化烯二酯、二醚、酯/醚及其混合物适宜作添加剂，二酯最好用窄沸点馏分，当少量单醚和单酯（它们常常在制造过程中生成）也可能存在时。少量二烷基化合物存在对于添加剂性能来说是重要的。特别是，聚乙二醇、聚丙二醇或聚乙二醇/聚丙二醇混合物的硬脂酸或二十二烷酸二酯是可取的。
在这一范畴内其他化合物的例子是在JPNos2-51477和3-34790（两者都是Sanyo公司的）和EP-A-117108和EP-A-326356（两者都是日本石油和脂肪公司）中描述的化合物。
乙烯/不饱和酯共聚物
例子是一种或多种乙烯和下列通式的不饱和单体的油溶性共聚物
Figure 921116446_IMG12
其中，R6是H或甲基，R5是-OOCR8基，R8是H或C1～C28（较好是C1～C17，最好是C1～C8）直链或支链烷基;或R5是-COOR8基，其中R8如以前描述的，但不是H，R7是H或-COOR8，如以前描述的。
当R6和R7是H，R5是-OOCR8时，单体包括C1～C29，特别是C1～C5单羧酸的乙烯基醇酯，最好是C2～C29，特别是C1～C5单羧酸的乙烯基醇酯和最好是C2～C5单羧酸的乙烯基醇酯。可与乙烯共聚的乙烯基酯的例子包括醋酸乙烯酯、丙酸乙烯酯和丁酸或异丁酸乙烯酯，醋酸乙烯酯是优选的。这些共聚物的数均分子量（用气相渗透压测定法测定）最好为1000～10000，最好是1000～5000。如果希望的话，共聚物由另外的共聚单体制得，它可为三聚物或四聚物或更高的聚合物，例如其中另一共聚物是异构烯烃，如二异丁烯。
极性有机含氮化合物
例子包括下列一个或多个化合物（a）～（c）。
（a）至少一摩尔烃基取代的胺与一摩尔有1～4个羧酸基的烃基酸或其酸酐反应生成的胺盐和/或酰胺;
可使用含30～300个（最好50～150个）碳原子的酯/酰胺。这些含氮化合物在US4211534中描述。适宜的胺一般是长链C12～C40伯胺、仲胺、叔胺或季胺或其混合物，但更短链胺也可使用，只要生成的含氮化合物是油溶性的，所以通常含大约30～300个碳原子。该含氮化合物最好含至少一个直链C8～C40，最好是C14～C24烷基段。
适宜的胺包括伯胺、仲胺、叔胺或季胺，但最好是仲胺。叔胺和季胺只可生成胺盐。胺的例子包括十四烷基胺、可可胺和氢化牛脂胺。仲胺的例子包括双-十八烷基胺和甲基-二十二烷基胺。胺混合物也是适宜的，如由天然物质制得的胺混合物。可取的胺是加氢牛脂仲胺，分子式为HNR1R2，其中R1和R2是由大约4%C14、31%C16、59%C18组成的加氢牛脂得到的烷基。
适合于制备含氮化合物的羧酸及其酐的例子包括环己烷1，2-二元羧酸、环己烷1，2-二元羧酸、环戊烷1，2-二元羧酸和萘二元羧酸。通常，这些酸在其环部分有5～13个碳原子。最适合用于本发明的酸是苯二元羧酸。如邻苯二甲酸、间苯二甲酸和对苯二甲酸。邻苯二甲酸或其酸酐是特别可取的。特别可取的化合物是通过1摩尔邻苯二甲酸酐与2摩尔二氢化牛脂胺反应生成的酰胺-胺盐、另一可取的化合物是由该酰胺-胺盐脱水生成的二酰胺。
其他例子包括如EP-A-327423中描述的缩合物。
（b）含环系的化学化合物，该化合物在环系上至少有下列通式（Ⅰ）的两个取代基
-A-NR1R2（Ⅰ）
其中A为被一个或多个杂原子任意间断的脂族烃基，它是直链烃基或支链烃基，R1和R2是相同的或不同的，每一个都含有被一个或多个杂原子任意间断的9～40个碳原子的烃基，取代基是相同的或不同的，该化合物可为其盐的形式。
A最好有1～20个碳原子，最好是亚甲基或聚亚甲基。
在本说明书中“烃基”指的是由氢和碳组成的有机部分，除非另加说明，它可能是包括环脂基在内的脂族基、芳族基或其组合基。它可为取代的或未取代的烷基、芳基或芳烷基、也可含不饱和基。被取代的基的例子是含氧、含卤和含羟烃基。
环系可包括均环、杂环，或稠环组合，或两个或两个以上这样的环相互连接。其中环组合可是相同的或不同的。当有两个或两个以上这样的环组合，通式（Ⅰ）的取代基可为相同的或不同的组合，最好是相同的组合。
每个环组合最好是芳族环，特别是苯环。
特别是，环系是单一的苯环时，取代基最好在邻位或间位，苯环可任意地再取代。
在环组合中环原子最好是碳原子，但例如也可包括一个或多个环上N、S或O原子，在这种情况下，该化合物是杂环化合物。
这样的多环组合的例子包括
·缩合苯结构，如萘、蒽、菲和芘;
·稠环结构，其中没有苯环或不全是苯环，如甘菊环、茚、氢茚、茐和联亚苯基;
·端连接环，如联苯;
·杂环化合物，如喹啉、吲哚、2，3-二氢吲哚、苯并呋喃、香豆素、异香豆素、苯并噻吩、咔唑和吩噻嗪;
·非芳族或部分饱和环系，如萘烷（即+氢化萘）、α-蒎烯、Cardinene和冰片烯;
·三维结构，如降冰片烯、双环庚烷（即降冰片烷）、双环辛烷和双环辛烯。
在本发明每一种含R1和R2的烃基（式Ⅰ）例如可为烷基或亚烷基或单一或多一烷氧烷基。每一基最好是直链烷基。在每一烃基中的碳原子数最好为16～40，特别是16～24。
环系最好只被两个通式为（Ⅰ）的取代基取代，A最好是亚甲基。
化学化合物盐的例子是醋酸酯和氯化氢。
化合物可方便地由相应的酰胺还原制得，酰胺可由仲胺与适当的酸性氯化物反应制得。
（c）长链伯胺或仲胺与含羧酸的聚合物的缩合物
具体的例子包括如GB-A-2121807、FR-A-2592387和DE-A-3941561中描述的聚合物;telemer酸和链烷醇胺的酯如US-A-4639256中描述的;含支链羧酸酯、环氧化物和单羧酸聚酯的胺的反应产物如在US-A-4631071中描述的。
烃类聚合物
例子为下列通式表示的聚合物
Figure 921116446_IMG13
其中，T为H或R1
U为H、T或芳基
V为1.0～0.0（摩尔比）
W为0.0～1.0（摩尔比）
其中R1为烷基。
这些聚合物可直接由乙烯属不饱和单体制得，或间接由单体（如异戊二烯、丁二烯等）制得的聚合物加氢制得。
烃类聚合物最好是乙烯和丙烯的共聚物，其乙烯含量最好为20～60重%，通常经均相催化剂制得。
烃类聚合物的例子在WO-A-9111488中描述。
羰基硫化合物
例子是EP-A-0261957中描述的，它描述了下式通式化合物的应用
Figure 921116446_IMG14
其中，-Y-R2为SO（-）（+） 3NR3 3R2、-SO（-）（+） 3HNR3 2R2、-SO3 （-）（+）H2NR3R2、-SO（-）（+） 3H3NR2、-SO2NR3R2或-SO3R2;-X-R1为-Y-R2或-CONR3R1、-CO（-）（+） 2NR3 3R2-CO（-）（+） 2HNR3 2R1、-R4-COOR1、-NR3COR1、-R4OR1、-R4OCOR1、-R4、-R1、-N（COR3）R1
或Z（-）（+）NR3 3R1;-Z（-）为SO（-） 3或-CO（-） 2;R1和R2为烷基烷氧基烷基或主链至少含10个碳原子的聚烷氧基烷基;R3为烃基，每-R3可为相同的或不同的和R4没有或为C1～C5亚烷基以及在
Figure 921116446_IMG15
中，碳碳键（C-C）或为a）乙烯属不饱和键（当A和B是烷基、烯基或取代的烃基），或b）部分环结构，它可为芳族环、稠环芳族环或环脂族环，最好是X-R1和Y-R2在其中含有至少三个烷基、烷氧烷基或聚烷氧烷基。
多组分添加剂体系可使用，所用各种添加剂的比例将取决于要处理的油品。
油料和燃料油
油料可为原油，即由钻井得到的炼制以前的石油，当本发明组合物可用作流动改进剂或脱蜡助剂时。
油料可为润滑油，润滑油可为动物油、植物油或矿物油，例如石油馏分（从石脑油或锭子油到润滑油）、蓖麻油、鱼油或氧化矿物油。本发明的添加剂组合物可用作润滑油的流动改进剂、降倾点剂或降蜡助剂。其他添加剂可在成品润滑油中存在，其他添加剂的例子是粘度指数改进剂、如乙烯-丙烯共聚物、琥珀酸基分散剂、含金属的分散添加剂和二烷基二硫代磷酸锌添加剂。
燃料油的例子是中间馏分油燃料油，即在原油炼制中得到的各种燃料油，如较轻的煤油和喷气燃料馏分和重燃料油馏分之间的馏分。例子是柴油燃料、航空燃料、煤油、燃料油、喷气燃料和取暖用油等。通常，适宜的馏分油燃料是沸点为120～500℃（ASTMD1160）的燃料，最好是150～400℃燃料，例如有相当高终馏点（FBP）（＞360℃）的燃料。燃料油可为动物油、植物油或矿物油。燃料油也可含其他添加剂，如稳定剂、分散剂、抗氧化剂、腐蚀抑制剂和/或破乳化剂。
取暖用油可由直馏馏分油（如瓦斯油、石脑油等）和裂化馏分油（如催化循环油）的调合油组成。柴油燃料代表性的规格包括最低闪点为38℃和90%馏出点为282～338℃（见ASTM    D-396和D-975）。
在本发明中，燃料中添加剂组合物的总量最好为0.0001～5.0重%，如0.001～0.5重%（活性物质），按燃料重量计。
本发明是一浓缩物，添加剂组合物可占20～90重%，如30～80重%。在浓缩物中使用的液体载体的例子是溶剂，如煤油、芳族石脑油和矿物润滑油。
实施例
本发明现在通过如下实施例详细地描述。正如将说明的那样，实施例除本发明的实施例外还包括对比实施例。 Mn指的是用GPC相对于聚苯乙烯标准测定的数均分子量。
添加剂
所用的添加剂如下，用所示的字母表示。
A：用于燃料Ⅰ和Ⅱ的测试（见下文），A是两种乙烯/醋酸乙烯酯共聚物的混合物：一种共聚物的数均分子量为2500，含36.5重%醋酸乙烯酯，每100个亚甲基含3-4个甲基;一种共聚物的 Mn为5000，含13.5重%醋酸乙烯酯，每100个亚甲基含6个甲基;两种共聚物的重量比为93∶7;为了进行保留燃料试验（见下文），A为乙烯/醋酸乙烯酯共聚物， Mn为3000，含29.0重%醋酸乙烯酯，每100个亚甲基含4个甲基。
B：一摩尔邻苯二甲酸酐与两摩尔二氢化牛脂胺的反应产物生成半酰胺/半胺盐。
D：单体通过用自由基催化剂制得的有16个碳原子的直链烷基的衣康酸酯的均聚物，均聚物的 Mn为3500。
G-K：一组苯乙烯/富马酸酯共聚物，其烷基有如下数字的碳原子，数均分子量为15000～30000
G    10
H    10～12
I    12
J    12～14
K    14
燃料油
所用的试验燃料油为燃料Ⅰ～Ⅵ，其特征列入下列图1，所有的温度为℃。
图1
燃料油
燃料油性质    I    II    III    IV    V    VI
浊点    -6    -5    -6    -7    -2    +3
基准CFPP    -8    -8    -9    -7    -4    0
D-86初馏点    166    168    135    136    178    179
20%    231    248    213    200    261    257
50%    276    279    277    248    291    293
90%    325    327    332    329    341    350
终馏点    348    358    361    364    368    373
试验温度    -17    -15    -17    -17    -15    -9
一般步骤
添加剂（它包括如所示单个添加剂组分通过添加剂符号字母搭配的组合物，结果见下文）用标准方法加到试验柴油燃料（1～Ⅵ），添加剂浓度对于A为200ppm（活性组分），对于B为200ppm（活性组分），对于所用的其他的每种添加剂组分为200ppm（活性组分）。然后对所处理的燃料进行如下试验。
低温过滤堵塞点试验（或CFPP试验）
通过在“Journal    of    the    Institute    of    Petroleum”第52卷、第510期173-285页（1966年6月）详细描述的步骤进行的试验用来关联车用柴油中中间馏分油的低温流动性。
简言之，40ml待处理的油样在浴中冷却（浴维持在大约-34℃），给出大约1℃/min的非线性冷却。周期地（在浊点以上开始的每一摄氏度），冷却油在规定的时间内，用试验设备进行通过细筛网流动性能的试验，该设备是一吸管，倒置的漏斗连接在它的底端，该漏斗置于待试验的油料表面下。漏斗口为12毫米直径确定的面积的350目筛。周期性试验每次通过在吸管上端抽真空开始，因此油料通过筛网被吸到吸管中到标明20毫升油料的刻度。每次成功通过后，油料立即返回CFPP管。每一度温降重复该试验，一直到油料不能在60秒内装满吸管为止，出现这一情况的温度作为CFPP温度。
抗蜡沉降试验（WAS）
沉降层的程度（WAS）用肉眼测量，作为留在测量烧瓶中经处理的燃料总体积的百分数。扩大的蜡沉降用低的数字表示，而未沉降的流体燃料用100%表示。有大量蜡结晶的胶凝的燃料的劣质样品几乎总是有高的数值;这样的结果因此记为“gel”。
结晶大小的测定
蜡结晶平均粒度用燃料样品的光学显微镜分析，以及在预定格子测定高达50个结晶的最长轴方法来测量。
结果
添加剂，或它们的组合在每一燃料Ⅰ-Ⅵ中被试验。在下列三张表的每张表中列出CFPP、WAS和结晶大小结果，分别称为表1、2和3。这里要提出下列说明
表1（CFPP）：所有结果℃都在0℃以下，即负值。
表2（WAS）：所有结果为分散的百分数，100为完全分散，在试验温度下2～3小时后进行观测。
表3（结晶大小）：所有值按1～10个分度，其中
10为＜10微米
9为10微米
8为10～20微米
7为20～50微米
6为50～100微米
5为100～200微米
4为200～300微米
3为300～500微米
2为500～700微米
1为＞700微米
从表1～3所示的结果可得出下列一般结论：
·添加剂AB（对比样）给出良好的总CFPP性能，但WAS和结晶大小性能不一致。
·添加剂ABD（对比样）给出良好的WAS和结晶大小性能，但CFPP变差。
上述变差可通过添加剂G-K中任何一种与ABD组合来补救，至少部分补救。
表1（CFPP）
燃料
添加剂    I    II    III    IV    V    VI    平均
AB    13    19    20    14    18    13    16.2
ABD    8    18    15    16    7    3    11.2
ABDG    11    19    17    15    15    7    14
ABDH    11    18    19    15    14    7    14
ABDI    11    18    20    15    14    10    14.7
ABDJ    10    17    20    16    15    9    14.5
ABDK    11    15    16    17    13    10    13.7
表2    (WAS)
燃料
添加剂    I    II    III    IV    V    VI    合计
AB    70    80    10    15    80    40    49.2
ABD    100    100    80    100    75    100    92.5
ABDG    95    40    100    100    100    20    75.8
ABDH    95    50    100    100    100    20    77.5
ABDI    95    50    100    100    100    20    77.5
ABDJ    95    50    95    100    100    80    86.7
ABDK    95    100    15    100    100    90    88.3
表3    (结晶大小)
燃料
添加剂    I    II    III    IV    V    VI    平均
AB    6    9    9    9    6    6    7.5
ABD    6    9    10    10    9    8    8.7
ABDG    6    9    10    10    7    6    8
ABDH    6    9    10    10    7    5    7.8
ABDI    6    9    10    10    7    6    8
ABDJ    6    9    10    10    9    5    8.2
ABDK    6    9    6    10    9    7    7.8

Claims (14)

1、一种添加剂组合物，它以组合的方式含有：
(i)一种含有下列结构单元的聚合物：
Figure 921116446_IMG2
其中，X为一整数，Y为0或一整数，在该聚合物中，X和Y的总和至少为2，结构单元(Ⅱ)与(Ⅰ)的比为0～2，结构单元(Ⅱ)与(Ⅲ)的比为0～2，其中
R1和R2是相同的或不同的，每一个代表一个C10～C30烷基，
R3代表H、-OOCR6、C1～C30烷基、-COOR6、-OR6、芳基或烷芳基或卤素
R4代表H或甲基
R5代表H、C1～C30烷基或-COOR6
R6代表C1～C22烷基
R1、R2、R3、…R4、R5和R6中的每一个都可任意被惰性取代，
(ii)一种梳型聚合物，在聚合物主链上有芳基和烃基，其中烃基有10个或10个以上碳原子。
2、一种权利要求1的组合物，其中组分（ⅱ）有下列通式：
Figure 921116446_IMG3
其中，D为R7、C（O）.OR、OC（O）.R7、R8C（O）.OR7或OR7
E为H或CH3或D或R8
G为H或D
m为1.0（均聚物）～0.4（摩尔比）
J为H、R8、芳基或杂环基、R8、CO.OR7
K为H、C（O）.OR8、OC（O）.R8、OR8、C（O）OH
L为H、R8、C（O）.OR8、OC（O）.R8、芳基、C（O）OH
n为0～0.6（摩尔比）
R7为含有10个或10个以上碳原子的烃基
R8为C1或更高的烃基，只要至少J和L中的一个是芳基。
3、权利要求1或2的组合物，其中如（ⅱ）确定的聚合物有下列通式
Figure 921116446_IMG4
其中，D、E、K和n如权利要求2中所规定的，J为一取代的或未取代的芳基。
4、权利要求3的组合物，其中聚合物是一种苯乙烯-马来酸酯共聚物或一种苯乙烯-富马酸酯共聚物。
5、权利要求4的组合物，其中马来酸酯或富马酸酯有含10～18个碳原子的烷基。
6、前面任何一项权利要求的组合物，其中组合物以组合方式含另一种馏分油燃料的低温流动改进剂。
7、前面任何一项权利要求组合物，其中如在（ⅰ）中定义的聚合物是一种二烷基衣康酸酯或二烷基柠康酸酯的均聚物，或是一种二烷基衣康酸酯或二烷基柠康酸酯与脂族烯烃、乙烯基醚、链烷酸的乙烯基酯、不饱和酸的烷基酯、芳族烯、乙烯基卤化物、二烷基富马酸酯或二烷基马来酸酯的共聚物。
8、前面任何一项权利要求的组合物，其中如（ⅰ）和（ⅱ）中定义的聚合物中的一个或两个的数均分子量为1000～50000。
9、权利要求8的组合物，其中聚合物的数均分子量为1000～20000。
10、一种原油、润滑油或燃料油组合物，该组合物含有大量原油、润滑油或燃料油和少量前面任何一项权利要求的添加剂组合物。
11、一种添加剂浓缩物，该浓缩物含分散在与原油、润滑油或燃料油相容的液体介质中的权利要求1～9中任何一种组合物的混合物。
12、权利要求1～9任何一项的添加剂组合物作为原油、润滑油或燃料油的流动改进剂或作为脱蜡助剂的应用。
13、权利要求10或12的应用或油料组合物，其中油料是中间馏分油燃料油。
14、一种改进原油、润滑油或燃料油流动性或帮助润滑油脱蜡的方法，该法包括权利要求1～9任何一项的添加剂组合物加到该油料中。
CN92111644A 1991-10-22 1992-10-21 添加剂组合物及其应用及含它们的燃料油组合物 Expired - Fee Related CN1038254C (zh)

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