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CN1031712A - 流动性改进剂和浊点降低剂 - Google Patents

流动性改进剂和浊点降低剂 Download PDF

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Publication number
CN1031712A
CN1031712A CN88106364A CN88106364A CN1031712A CN 1031712 A CN1031712 A CN 1031712A CN 88106364 A CN88106364 A CN 88106364A CN 88106364 A CN88106364 A CN 88106364A CN 1031712 A CN1031712 A CN 1031712A
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alkyl
carbon atoms
ester
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polymkeric substance
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CN1025045C (zh
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卢泰斯·肯尼思
布兰德·贾克莱恩
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ExxonMobil Chemical Patents Inc
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Exxon Chemical Patents Inc
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Abstract

适用于改善原油、润滑油、尤其是燃料油的流动 性和/或降低其浊点的添加剂为含有其链长至少为 8个碳原子的烷基的聚合物。该聚合物为(a)仅含有 两个烷基的单体化合物，其中之一比另一个烷基至少 多含3个碳原子或(b)仅含有三个烷基的单体混合 物，其中烷基间链长之差至少为3个碳原子，中长链 的烷基链长为其它二者链长之和的一半。该聚合物 也可由含有两个上述定义烷基的单体(a)或含有三个 上述定义烷基的单体(b)来制备。

Description

本发明涉及特别适用于燃料油，尤其是馏分燃料油的流动性改进剂和浊点降低剂。
已经提出了多种浊点降低剂（即在温度降低时抑制燃料油中产生蜡结晶的添加剂），且这些浊点降低剂也是有效的。然而，业已发现，当将这些浊点降低剂在燃料油中与流动性改进剂一起使用时，流动性改进剂的性能将遭到破坏。
本发明人找到了不仅可作为有效的浊点降低剂、且对可加入燃料油中的其它流动性改进剂的性能没有实际不利影响的浊点降低剂。
而且，本发明的聚合物单独使用或与其它已知添加剂一起使用时也是有效的馏分燃料流动性改进剂。其应用可扩展到其中的蜡随环境温度下降而沉淀，从而引起流动性问题的燃料和油品，例如应用于喷气燃料、煤油、柴油、加热炉燃料、燃料油品、原油和润滑油。这些聚合物也用作蜡晶调节剂以改变蜡晶的大小和形状，从而改善燃料或油品的低温流动性（低温过滤阻塞试验（CFPP），IP309/80测定）。还能用来控制蜡开始结晶的温度（浊点试验，IP    219    ASTM    D2500测定）。
本发明的浊点降低剂和/或流动性改进剂包括：
（1）下述（a）或（b）的混合物生成的聚合物：
（a）含有一个烷基的单体，所述烷基至少有8个碳原子，大体上只有两个长度不同的链，且其中一个链比另一个至少长3个碳原子，
（b）含有一个烷基的单体，所述烷基至少有8个碳原子，大体上只有三个长度不同的链，且这些链长之差至少为3个碳原子;或
（2）下述单体（c）或（d）的聚合物：
（c）大体上只有两个烷基的单体，所述烷基至少有8个碳原子，且其中一个烷基比另一个至少长3个碳原子，
（d）大体上只有三个烷基的单体，所述烷基至少有8个碳原子，且每一烷基与其它烷基至少相差三个碳原子;
上述单体可根据需要与间隔单体共聚。
重要的是，如果上述定义的任何烷基是支链化的，每一烷基的支链必须不多于一个甲基。
若聚合物是由有三个烷基的单体形成的，中长链的烷基最好是短链和长链烷基链长总和的一半。
以本文所述的方式作用于蜡的聚合物可被描述为“梳形”聚合物，即主链上悬挂有烷基侧链的聚合物。由于本发明的聚合物包括在同一聚合物上混合两个侧链，这些侧链可以在单体成型之间引入（如单体可含有两个侧链）或将具有各自侧链长度不同的单体混合，形成单体混合物。
本发明还提供了使用
（1）下述（a）或（b）的混合物生成的聚合物：
（a）含有一个烷基的单体，所述烷基至少有8个碳原子，大体上只有两个长度不同的链，且其中一个链比另一个至少长3个碳原子，
（b）含有一个烷基的单体，所述烷基至少有8个碳原子，大体上只有三个长度不同的链，且这些链长之差至少为3个碳原子;或
（2）下述单体（c）或（d）的聚合物：
（c）大体上只有两个烷基的单体，所述烷基至少有8个碳原子，且其中一个烷基比另一个至少长3个碳原子，
（d）大体上只有三个烷基的单体，所述烷基至少有8个碳原子，且每一烷基与其它烷基至少相差三个碳原子;
上述单体可根据需要与间隔单体共聚，
来降低燃料油的浊点和/或改善其流动性的方法。
重要的是，如果上述定义的任何烷基是支链化的，其支链必须不多于一个甲基。
应再次指出，若聚合物是由有三个甲基的单体形成的，中长度的烷基的链长最好是短链和长链烷基链长总和的一半。
“大体上只有两个烷基”或“大体上只有三个烷基”意指至少90%的烷基应是所定义的烷基。
可以采用范围广泛的聚合物混合物或聚合物，条件是这些聚合物具有上述定义数量和大小的烷基。例如，可以使用富马酸二烷酯-乙酸乙烯酯、衣康酸烷酯-乙酸乙烯酯共聚物或衣康酸烷酯、丙烯酸烷酯、异丁烯酸烷酯和α-烯烃聚合物的混合物。由此可见，“间隔”基（例如乙酸乙烯酯）可被插入聚合物，且这些基不受上述定义的链长限制。
单体混合物或聚合物中限定的烷基必须含有至少8个碳原子。较好的是有10-20个碳原子，且适当的二组合为C10和C14，C12和C10，以及C14和C18;较好的三组合为C10，C14和C18，C11，C14和C17，C12，C15和C18。较好的烷基是正烷基，但必要时也可使用支链烷基。若有侧链，则甲基侧链只能有一个，如在主链的1或2位上，例如1-甲基十六烷基。
较好的是，烷基链长的差别至少为5个碳原子，特别是对于有两个或三个不同烷基的单体的聚合物。
聚合物和聚合物混合物中聚合物的数均分子量可以彼此不同，但一般为1000-500，000，较好的为2000-100，000（凝胶渗透色谱法测定）。
典型的聚合物是含有25-100%（重量），较好的为约50%（重）的二元羧酸和0-75%（重），较好的为约50%（重）的α-烯烃或其它不饱和酯（如乙烯基酯和/或丙烯酸烷酯或异丁烯酸烷酯）的共聚物。特别好的是富马酸二正烷酯的均聚物或富马酸二正烷酯和乙酸乙烯酯的共聚物。
适用于制备优选聚合物的单体（如羧酸酯）可用下面的通式表示：
Figure 881063649_IMG1
其中R1和R2是氢或C1-C4烷基（如甲基），R3是R5、COOR5、OCOR5或OR5，R4是COOR3、氢或C1-C4烷基，较好的是COOR3，R5是C1-C22烷基或取代的C1-C22芳基。这些单体可以通过用适当的醇或醇混合物酯化特定的一或二元羧酸来制备。
其它可以共聚的不饱和酯的实例有丙烯酸烷酯和异丁烯酸烷酯。二羧酸单或双酯单体可与不同量的[如5-75%（摩尔）]其它不饱和酯或烯烃共聚。这里所说的其它酯包括具有下式的短链烷基酯：
Figure 881063649_IMG2
其中R′是氢或C1-C4烷基，R″是-COOR″″或-OCOR″″（其中R″″是支链或非支链C1-C5烷基），R″′是R″或氢。这些短链酯的实例有异丁烯酸酯，丙烯酸酯，乙烯酯，例如乙酸乙烯酯和丙烯乙烯酯（以丙酸乙烯酯为佳）。更具体的实例包括异丁烯酸甲酯，乙酸异丙烯酯和丙烯酸丁酯和丙烯酸异丁酯。
较好的共聚物含有40-60%（摩尔）富马酸二烷酯和60-40%（摩尔）乙酸乙烯酯，其中富马酸二烷酯中的烷基如前所定义。
若使用酯的聚合物或共聚物，可用下述聚合方法方便地进行制备：在一种烃类溶剂（如庚烷、苯、环己烷或白油）的溶液中，在惰性气氛下（如氮气或二氧化碳），以20-150℃的温度聚合酯单体，聚合中通常采用过氧化物或偶氮型催化剂（如过氧化苯甲酰或偶氮二异丁腈）作促进剂。
宜于互相二组合的单体的具体实例有：
富马酸二-十二烷酯和富马酸二-十八烷酯;
富马酸二-十三烷酯和富马酸二-十九烷酯;
马来酸二-十二烷酯和马来酸二-十八烷酯与苯乙烯;
衣康酸二-十三烷酯和衣康酸二-十八烷酯;
衣康酸二-十四烷酯和衣康酸二-十八烷酯;
衣康酸二-十二烷基酯和衣康酸二-十八烷基酯;
衣康酸十四烷酯和衣康酸二-二十烷酯;
丙烯酸癸酯和丙烯酸十六烷酯;
丙烯酸十三烷酯和丙烯酸十九烷酯;
异丁烯酸癸酯和异丁烯酸十八烷酯;
1-十二碳烯和1-十六碳烯;
1-十四碳烯和1-十八碳烯。
以上成对的单体可以与间隔单体（如乙酸乙烯酯）一起聚合。
除上述二烷基化合物外，还可以使用一烷基等同物，例如富马酸十二烷酯和富马酸十八烷酯聚合物。
宜于互相三组合的单体的具体实例有：
富马酸二-十二烷酯、富马酸二-十五烷酯和富马酸二-十八烷酯;
富马酸二癸酯、富马酸二-十四烷酯和富马酸二-十八烷酯与乙酸乙烯酯;
富马酸二癸酯、马来酸二-十四烷酯和马来酸二-十八烷酯与苯乙烯;
衣康酸二-十三烷酯、衣康酸二-十六烷酯和衣康酸二-十九烷酯与乙酸乙烯酯;
衣康酸二-十二烷酯、衣康酸二-十六烷酯和衣康酸二-二十烷酯;
丙烯酸癸酯、丙烯酸十五烷酯和丙烯酸二十烷酯;
异丁烯酸十二烷酯、异丁烯酸十六烷酯和异丁烯酸二十烷酯;
1-十二碳烯、1-十五碳烯和1-十八碳烯。
有三个不同烷基的适宜的聚合物的具体实例有富马酸正癸酯、富马酸正十四烷酯和富马酸正十八烷酯-乙酸乙烯酯共聚物。
在酯化或烷基化苯环时，通过采用适宜链长的醇的混合物，可以方便地制备有两个或三个不同烷基的聚合物。
一般来说，较好的是采用富马酸二烷酯-乙酸乙烯酯共聚物或富马酸二烷酯聚合物，具体讲是富马酸二癸酯-富马酸二-十八烷酯-乙酸乙烯酯共聚物，富马酸二-十二烷酯-富马酸二-十六烷酯-乙酸乙烯酯共聚物，富马酸十二烷基十六烷基二酯-乙酸乙烯酯共聚物，富马酸二癸酯和富马酸二-十八烷酯聚合物，富马酸十二烷酯-富马酸二-十六烷酯聚合物，富马酸十二烷基十六烷基二酯聚合物。α-烯烃聚合物的实例有十二碳烯、二十碳烯共聚物和十四碳烯/十八碳烯共聚物。
本发明的添加剂可以加到燃料油（如液体烃类燃料油）中。液体烃类燃料油可以是馏分燃料油如中间馏分燃料油（例如柴油、航空燃料、煤油、燃油、喷气燃料、加热炉油）等。合适的馏分燃料通常是那些沸程为120℃-500℃（ASTM    D86），较好的是那些沸程为150℃-400℃的馏分（如沸程为120℃-500℃的石油馏分燃料），或其中90%油品的沸点至终沸点10-40℃且终沸点为340℃-400℃的馏分。加热油较好的是直馏馏分（如粗柴油、石脑油等）和裂化馏分（如催化循环油料）的调制品。本发明的添加剂也可加到原油或润滑油中。
添加剂的添加量只占很小的比例，一般为燃料油重量的0.0001-0.5%，较好的为0.001-0.2%，特别好的为0.01-0.05%（活性物质）。
一般来讲，当加入了本发明的添加剂的燃料组合物掺有其它已知的改善馏分燃料低温流动添加剂时，常常取得更好的效果。这些已知添加剂的实例有聚氧亚烷基酯、醚、酯/醚、酰胺/酯及其混合物，特别是那些分子量为100-5000（最好为200-5000）的聚氧亚烷基乙二醇中含有至少一个、最好至少两个C10-C30线型饱和烷基的添加剂，其中所述聚氧亚烷基乙二醇中的烷基含有1-4个碳原子。欧洲专利公开0，061，895叙述了某些这种添加剂。
较好的酯、醚或酯/醚的结构可由下式表示：
R5-O-（A）-O-R6
其中R5和R6可相同或不相同，可以是
（ⅰ）正烷基
（ⅱ）正烷基
Figure 881063649_IMG3
（ⅲ）正烷基
Figure 881063649_IMG4
（ⅳ）正烷基
Figure 881063649_IMG5
烷基是直链饱和的、且含有10-30个碳原子;A表示二醇的聚氧亚烷基部分，其中的亚烷基有1-4个碳原子，如聚氧亚甲基、聚氧亚乙基或聚氧三亚甲基部分;可以允许某种程度的低级烷基侧链的支化（如在聚氧亚丙基二醇中），但是基本上是直链的二醇是优选的。
适宜的二醇一般是分子量为约100-5000，最好为200-2000的、基本上直链的聚乙二醇（PEG）和聚丙二醇（PPG）。酯是优选的，含有10-30个碳原子的脂肪酸可用于与二醇反应形成酯添加剂。较好的是使用C18-C24脂肪酸，特别是山萮酸。酯也可以通过酯化聚乙氧基化的脂肪酸或醇来制备。这种类型特别优选的添加剂是聚二山萮酸乙二醇酯，二醇部分的分子量约为600，常简称为PEG600二山萮酸酯。
其它与本发明的浊点降低剂一起使用的适宜添加剂是乙烯不饱和酯共聚物流动性改进剂。可与乙烯共聚的不饱和单体包括下面通式所示的不饱和的单酯或双酯：
Figure 881063649_IMG6
其中R8是氢或甲基，R7是-OOCR10（R10是氢或C1-C28通常为C1-C17、最好为C1-C8直链或支链烷基），或是-COOR10（R10如上所定义，但不是氢），R9是氢或如上定义的-COOR10。当R7和R9是氢且R8是-OOCR10时，单体包括C1-C29一元羧酸的乙烯醇酯，通常为C1-C29一元羧酸，更常见的为C1-C18一元羧酸，较好的是C2-C29一元羧酸，更常见的为C1-C18一元羧酸，最好是C2-C5一元羧酸。可与乙烯共聚的乙烯基酯的实例有乙酸乙烯酯，丙烯乙烯酯和丁酸乙烯酯或异丁酸乙烯酯，以乙酸乙烯酯为佳。较好的是含有20-40%（重）乙酸乙烯酯，更好的是含有25-35%（重）乙酸乙烯酯的共聚物。这些添加剂也可以是两种共聚物的混合物，如USP3，961，916所述。这些共聚物的数均分子量（气相渗透压力测定法）一般为1000-6000，以1000-30000为好。
其它适于与本发明的添加剂一起使用的添加剂是离子的或非离子的极性化合物，它们在燃料油中有抑制蜡晶生长的能力。极性含氮化合物与二醇酯、醚或酯/醚组合使用特别有效。这些极性化合物通常是由至少1摩尔烃基取代的胺与1摩尔具有1-4个羧酸基的烃基酸或其酐反应形成的胺盐和/或酰胺。也可以使用含有总数把30-300，较好的为50-150个碳原子的酯/酰胺。USP4，211，534叙述了这些氮化合物。适用的胺通常是长链C12-C40伯、仲、叔或季胺或其混合物，若生成的氮化合物是油溶的，因而一般含有总数为30-300个碳原子，也可以采用较短链的胺。氮化合物最好含有至少一个C8-C40直链烷基，以C14-C24烷基为好。
适用的胺包括伯胺、仲胺、叔胺或季胺，以仲胺为好。叔胺和季胺只能形成胺盐。胺的实例包括十四烷胺，可可胺，氢化动物脂胺等。仲胺的实例包括二-十八烷胺，甲基-山萮胺等。胺混合物也是适用的，由天然材料衍生的许多胺都是混合物。较好的胺是式为HNR1R2的氢化牛脂胺，其中R1和R2是由氢化动物脂衍生的、由大约4%C14、31%C1659%C18构成的烷基。
适于制备这些氮化合物（及其酐）的羧酸的实例包括环己烷1，2-二羧酸，环己烷二羧酸，环戊烷1，2-二羧酸，萘二甲酸等。
这些酸在其环部分一般有5-13个碳原子。较好的酸是苯二羧酸，例如苯二甲酸、对苯二酸和间苯二酸。苯二甲酸及其酐是特别可取的。特别好的化合物是由1摩尔苯二甲酸酐与2摩尔二氢化动物脂胺反应形成的酰胺/胺盐。另一较好的化合物是这种酰胺-胺盐脱水形成的二酰胺。
添加剂混合物中，较好的是使用0.05-20份（重），更好的是0.1-5份（重）本发明的添加剂，1份（重）其它添加剂如聚氧亚烷基酯、醚或酯/醚或酰胺/酯。
可以方便地将本发明的添加剂溶于适当溶剂，制成含20-90%（重），例如30-80%（重）聚合物的浓缩物。适用的溶剂包括煤油，芳族石脑油，矿物润滑油等。
实施例1
在该实施例中使用三种本发明的添加剂。第一种（CDⅠ）为50%（摩尔）富马酸正癸基正十八烷基二酯与50%（摩尔）乙酸乙烯酯的共聚物，其数均分子量为35000。第二种添加剂（CD2）为50%（摩尔）富马酸正十二烷基正十六烷基二酯与50%（摩尔）乙酸乙烯酯的共聚物，其数均分子量为35000。第三种添加剂（CD3）为由25%（摩尔）富马酸正二（十六烷基）酯、25%（摩尔）富马酸正二（十二烷基）酯的混合物和50%（摩尔）乙酸乙烯酯的共聚物，其中富马酸酯于酯化后相互混合。该共聚物的数均分子量为31200。
在加至各种燃料中时，每种添加剂以1∶4的重量比与含有乙烯/乙酸乙烯酯共聚物的混合物的流动性改进剂K混合。上述乙烯/乙酸乙烯酯共聚物的混合物由含有36%乙酸乙烯酯且数均分子量为约2000的乙烯/乙酸乙烯酯共聚物与含有13%（重量）乙酸乙烯酯且数均分子量约为3000的乙烯/乙酸乙烯酯共聚物以3∶1重量比的混合物。
为了测试这些添加剂作为流动性改进剂和浊点降低剂的效力，将它们以0.010-0.0625%（重量，活性物质）的浓度加至具有下列特性的七种不同燃料A-G中：
ASTM-D86蒸馏
WAT    CP    CFPP    初沸点    20%    50%    80%    90%    初沸
点
A    1    2    1    184    270    310    338    350    369
B    2    6    2    173    222    297    342    356    371
C    -6    0    -3    190    246    282    324    346    374
D    1    4    -3    202    263    297    340    360    384
E    -1    1    -1    176    216    265    318    340    372
F    0    3    0    188    236    278    326    348    376
G    0    3    0    184    226    272    342    368    398
先后对燃料自身及含有添加剂的燃料进行低温过滤堵塞点试验并用差示扫描量热法进行测定，其详细情况如下所示：
低温过滤堵塞点试验（CFPPT）
通过低温过滤堵塞点试验（CFPPT）测定混合物的低温流动性。该试验采用《Journal of the Iustitute of Petroleum》卷52，No.510，1966年6月，第173-185所详述的步骤进行。简言之，借助保持在-34℃的浴冷却140ml待试验的油样。周期性地（由浊点以上2℃开始每降温1℃）测试冷却油在一定时间内流过一细网的能力。将一个位于待测试油表面之下的倒置漏斗与吸管的下端连接在一起，采用如此构成的设置测试上述低温性能。漏斗口上铺盖有面积约为0.45平方英寸的350目筛网。每次周期性试验开始时都是使吸管的上端形成真空以便将油（20ml）经筛网吸至吸管之中。每降温一度重复一次试验，直至60秒内油不能充入吸管内为止。试验结果以CFPP（℃）表示，它表示未经处理的燃料（CFPP0）与经过流动改进剂处理的燃料（CFPP1）之间的温差，即△CFPP＝CFPP0-CFPP1。
在DSC（差示扫描量热法）中，测定的以℃表示的△WAT（蜡出现温度）是将25ml油样置于热量计中以2℃/分钟的速率冷却，只有基础馏分的燃料出现蜡时的温度（WAT0）与经过处理的馏分燃料油出现蜡时的温度（WAT1）之差，即△WAT＝WAT0-WAT1。
在这些研究中所用的仪器为Metler    TA2000B。业已发现，△WAT值与浊点降低有关。
测定的还有CFPP回归，这一数值为经过流动性改进剂（例如聚合物混合物K）单独处理的燃料的CFPP值与经过流动改进剂（例如聚合物混合物K）和浊度降低剂处理的燃料的CFPP1值之差。CFPP回归值越小，则浊点降低剂对流动性改进剂性质的不利影响越小。CFPP回归值＝CFPP（流动改进剂K）-CFPP（浊点降低剂）。若CFPP回归值为负数，则意味着CFPP值得到提高。
每种燃料的△CFPP值及CFPP回归值均测两次，其平均值如下表示。
Figure 881063649_IMG7
为了进行对比，采用分别为富马酸二（十四烷基）酯/乙酸乙烯酯共聚物、富马酸二（C14/C16烷基）酯/乙酸乙烯酯共聚物（醇在用富马酸酯化前相互混合）以及富马酸二（十六烷基）酯/乙酸乙烯酯共聚物的X、Y和Z三种富马酸二烷基酯/乙酸乙烯酯共聚物代替CD1、CD2和CD3，对同种燃料进行同一试验。在每种共聚物中，含有50%（摩尔）乙酸乙烯酯，共聚物的数均分子量约为4200。
Figure 881063649_IMG8
可以看出，与上述已知的富马酸二烷基酯/乙酸乙烯酯共聚物X、Y和Z相比，本发明浊点降低剂CD1、CD2和CD3的△CFPP、CFPP回归值和△WAT均较好。
实施例2
在本实施例中，使用CD4、CD5和CD6三种聚富马酸二烷基酯作为流动性改进剂和浊点降低剂。
CD4为数均分子量约为4200的聚富马酸（正癸基/正十八烷基）二酯，CD5为数均分子量约为3300的聚富马酸（正十二烷基/正十六烷基）二酯，CD6为富马酸二（正十六烷基）酯和富马酸二（正十二烷基）酯的混合物（1∶1摩尔）的共聚物，其数均分子量为4300。
使用实施例1所用的流动性改进剂（即聚合物混合物K）。每种浊点降低剂以1∶4的摩尔比与流动性改进剂混合。
为了测试与流动改进剂结合使用的浊点降低剂的效力，将其以相同的浓度加至用于实施例1的七种燃料A-G之中。
先后对燃料自身和含有添加剂的燃料进行低温过滤堵塞点试验并采用差示扫描量热法进行测定。结果如下所示。
为了进行对比，还在燃料G中对下列聚富马酸酯进行了试验
PF1    聚富马酸（正十二烷基/正十四烷基）二酯
PF2    聚富马酸正十四烷基酯和
PF3    聚富马酸（正十四烷基/正十六烷基）二酯。
Figure 881063649_IMG9
一般情况下，上述结果优于采用实施例1所示先有技术添加剂X、Y和Z以及采用产品PF1、PF2和PF3所获得的结果。
实施例3
在本实施例中，制备特定的聚α-烯烃并将其加至实施例1的燃料A、C和G之中，对流动改进活性及浊点降低进行测定。在某些试验中还加入了实施例1的流动性改进剂。
其中聚α-烯烃为：
P：十二碳烯/二十碳烯共聚物
Q：十四碳烯/十八碳烯共聚物
在每种情况下，两种单体的摩尔比均为1∶1。
试验为CFPP和DSC。
试验结果如下所示：
DSC条件：2℃/分    冷却速率
20    uV    fsd（满刻度偏转）
以煤油作为参考物
25    ul试样
由+20℃冷却至-20℃
WAT℃    △WAT℃
燃料    A自身    -3.7
500ppm    P    -6.6    2.9
500ppm    Q    -6.1    2.4
DSC条件：2℃/分    冷却速率
20    uV    fsd（满刻度偏转）
以煤油作为参考物
25    ul    试样
由+20℃冷却至-20℃
WAT℃    △WAT℃
燃料    C    自身    -6.0
500ppm    P    -9.7    3.7
500ppm    Q    -9.6    3.6
还采用燃料G测试以更为常见方法制备的聚α-烯烃。
例如：
R＝聚α-十四碳烯
S＝聚α-十六碳烯
T＝聚α-十八碳烯
U＝聚α-二十碳烯
将其试验结果与本发明聚合物的结果对比。
DSC条件：2℃/分    冷却速率
20    uV    fsd（满刻度偏转）
以煤油作为参考物
25    ul    试样
由+20℃冷却至-20℃
Figure 881063649_IMG14
所获得的结果一般情况下优于采用实施例1所示先有技术添加剂X、Y和Z所得到的结果。
实施例4
将两种苯乙烯/马来酸酯共聚物M和N（同流动改进剂K一样）以各种浓度加至实施例1的燃料G之中。共聚物M为苯乙烯与马来酸（正癸基/正十八烷基）二酯的等摩尔混合物的共聚物，共聚物N为苯乙烯与马来酸（正十二烷基/正十六烷基）二酯的等摩尔混合物的共聚物。
试验为CFPP和DSC。试验结果如下所示：
Figure 881063649_IMG15
还采用燃料G测试采用更为常见方法制备的苯乙烯/马来酸酯共聚物。
例如：
V＝苯乙烯-马来酸二（正癸基）酯共聚物
W＝苯乙烯-马来酸二（正十二烷基）酯共聚物
X＝苯乙烯-马来酸二（正十四烷基）酯共聚物
Y＝苯乙烯-马来酸二（正十六烷基）酯共聚物
Z＝苯乙烯-马来酸二（正十八烷基）酯共聚物
其△CFPP和△WAT结果与由共聚物M和N得到的结果对比，可以看出，采用本发明共聚物一般情况下所获得的总体结果最佳。
Figure 881063649_IMG16
DSC条件：2℃/分    冷却速率
20    uV    fsd（满刻度偏转）
以煤油作为参考物
25    ul    试样
由+20℃冷却至-20℃
Figure 881063649_IMG17
一般情况下，其结果优于采用实施例1所示先有技术添加剂X、Y和Z所得到的结果。

Claims (30)

1、一种适用于燃料油、原油或润滑油的添加剂，包括
(1)下述(a)或(b)的混合物生成的聚合物：
(a)含有一个烷基的单体，所述烷基至少有8个碳原子，大体上只有两个长度不同的链，且其中一个链比另一个至少长3个碳原子，
(b)含有一个烷基的单体，所述烷基至少有8个碳原子，大体上只有三个长度不同的链，且这些链长之差至少为3个碳原子；或
(2)下述单体(c)或(d)的聚合物：
(c)大体上只有两个烷基的单体，所述烷基至少有8个碳原子，且其中一个烷基比另一个至少长3个碳原子，
(d)大体上只有三个烷基的单体，所述烷基至少有8个碳原子，且每一烷基与其它烷基至少相差三个碳原子；
上述单体可根据需要与间隔单体共聚。
2、按照权利要求1所述的添加剂，其中聚合物由基本上仅含有三个烷基的单体制得，在该单体的三个烷基之中，中长链的烷基链长为最长与最短两个烷基链长之和的一半。
3、按照权利要求1或2所述的添加剂，其中所述烷基含有10-20个碳原子，该烷基以正烷基为佳。
4、按照上述任一权利要求所述的添加剂，其中所述烷基间的链长之差至少为5个碳原子。
5、按照上述任一权利要求所述的添加剂，其中根据凝胶渗透色谱测得的聚合物的数均分子量在1000-500000范围内。
6、按照上述任一权利要求所述的添加剂，其中聚合物为含有25-100%（重量）二羧酸二正烷基酯和0-75%（重量）α-烯烃或另一种不饱和酯的共聚物。
7、按照权利要求6所述的添加剂，其中添加剂为富马酸二正烷基酯的均聚物或富马酸二正烷基酯与乙酸乙烯酯的共聚物。
8、按照权利要求7所述的添加剂，其中共聚物含有40-100%（摩尔）富马酸二羧酸二正烷基酯及60-0%（摩尔）乙酸乙烯酯。
9、一种组合物，其中含有原油、燃油或润滑油和小比例（重）的上述任一权利要求所述的添加剂。
10、按照权利要求9所述的组合物，其中燃料油是沸程为120-500℃（ASTM  D86）的馏分燃料。
11、按照权利要求9或10所述的组合物，其中以燃料油重量为基准计，添加剂含量为0.0001-0.5%（重量，活性物质），以0.001-0.2%为佳。
12、按照权利要求9-11中任一项所述的组合物，其中还包括聚氧化亚烷基酯、醚、酯/醚、酰胺/酯或其混合物。
13、按照权利要求9-12中任一项所述的组合物，其中还包括作为流动改进剂的乙烯/不饱和酯共聚物，以乙烯/乙酸乙烯酯共聚物为佳。
14、按照权利要求9-13中任一项所述的组合物，其中还包括抑制燃料中蜡晶生长的离子或非离子型极性化合物，以含氮极性化合物如胺盐和/或酰胺为佳。
15、应用下列聚合物：
（1）下述（a）或（b）的混合物生成的聚合物：
（a）含有一个烷基的单体，所述烷基至少有8个碳原子，大体上只有两个长度不同的链，且其中一个链比另一个至少长3个碳原子，
（b）含有一个烷基的单体，所述烷基至少有8个碳原子，大体上只有三个长度不同的链，且这些链长之差至少为3个碳原子;或
（2）下述单体（c）或（d）的聚合物：
（c）大体上只有两个烷基的单体，所述烷基至少有8个碳原子，且其中一个烷基比另一个至少长3个碳原子，
（d）大体上只有三个烷基的单体，所述烷基至少有8个碳原子，且每一烷基与其它烷基至少相差三个碳原子;
上述单体可根据需要与间隔单体共聚，
作为燃料油的浊点降低剂和/或流动性改进剂。
16、按照权利要求15所述的用途，其中聚合物由基本上仅含有三个烷基的单体制得，在该单体的三个烷基之中，中长链的烷基链长为最长与最短两个烷基链长之和的一半。
17、按照权利要求15或16所述的用途，其中所述烷基含有10-20个碳原子，以正烷基为佳。
18、按照权利要求15-17中任一项所述的用途，其中所述烷基间的链长之差至少为5个碳原子。
19、按照权利要求15-18中任一项所述的用途，其中根据凝胶渗透色谱测得的聚合物的数均分子量在1000-500000范围内，以2000-100000为佳。
20、按照权利要求15-19中任一项所述的用途，其中聚合物为含有25-100%（重量）二羧酸二正烷基酯和0-75%（重量）α-烯烃或另一种不饱和酯的共聚物。
21、按照权利要求20所述的用途，其中聚合物为富马酸二正烷基酯的均聚物或富马酸二正烷基酯与乙酸乙烯酯的共聚物。
22、按照权利要求21所述的用途，其中共聚物含有40-100%（摩尔）富马酸二烷基酯和60-0%（摩尔）乙酸乙烯酯。
23、一种浓缩物，其中含有10-80%（重）溶剂和20-90%（重量）的、
（1）下述（a）或（b）的混合物生成的聚合物：
（a）含有一个烷基的单体，所述烷基至少有8个碳原子，大体上只有两个长度不同的链，且其中一个烷基比另一个至少长3个碳原子，
（b）含有一个烷基的单体，所述烷基至少有8个碳原子，大体上只有三个长度不同的链，且这些链长之差至少为3个碳原子;或
（2）下述单体（c）或（d）的聚合物：
（c）大体上只有两个烷基的单体，所述烷基至少有8个碳原子，且其中一个烷基比另一个至少长3个碳原子，
（d）大体上只有三个烷基的单体，所述烷基至少有8个碳原子，且每一烷基与其它烷基至少相差三个碳原子;
上述单体可根据需要与间隔单体共聚。
24、按照权利要求23所述的浓缩物，其中聚合物由基本上仅含有三个烷基的单体制得，在该单体的三个烷基中，中长链的烷基链长为最长与最短两个烷基链长之和的一半。
25、按照权利要求23或24所述的浓缩物，其中所述烷基含有10-20个碳原子，该烷基以正烷基为佳。
26、按照权利要求23-25中任一项所述的浓缩物，其中所述烷基间的链长之差至少为5个碳原子。
27、按照权利要求23-26中任一项所述的浓缩物，其中根据凝胶渗透色谱测得的聚合物的数均分子量在1000-500000范围内。
28、按照权利要求23-27中任一项所述的浓缩物，其中聚合物为含有25-100%（重量）二羧酸二正烷基酯和75-0%（重量）α-烯烃或另一种不饱和酯的共聚物。
29、按照权利要求28所述的浓缩物，其中共聚物由富马酸二正烷基酯与乙酸乙烯酯的共聚物。
30、按照权利要求29所述的浓缩物，其中共聚物含有40-60%（摩尔）富马酸二烷基酯和60-40%（摩尔）乙酸乙烯酯。
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