CN111349461A - 油防结垢和/或防沥青质附聚法 - Google Patents
油防结垢和/或防沥青质附聚法 Download PDFInfo
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- CN111349461A CN111349461A CN201911249047.0A CN201911249047A CN111349461A CN 111349461 A CN111349461 A CN 111349461A CN 201911249047 A CN201911249047 A CN 201911249047A CN 111349461 A CN111349461 A CN 111349461A
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Abstract
本公开涉及通过在油中提供一种添加剂组合减轻在烃油的中游工艺和运输以及上游运输中的结垢和/或沥青质附聚(或絮凝),所述添加剂组合包含:(A)聚烯基取代的羧酸或酐,和(B)金属清净剂体系,其包含烃基取代的羟基苯甲酸金属盐、或烃基取代的磺酸金属盐或这两种盐的混合物或所述盐的络合物,其中(A)与(B)的质量:质量比在20:1至1:20的范围内且所述添加剂的处理率在5至10000质量ppm的范围内。
Description
发明领域
本发明涉及用于减轻在烃油(特别是原油)的中游工艺和运输以及上游运输中的结垢和/或沥青质附聚(或絮凝)的添加剂。
技术背景
沥青质包括大量结构,如具有杂原子的高分子量稠合芳族化合物;它们是主要由碳和氢构成但也含有次要组分如硫、氧、氮和各种重金属的杂环不饱和大分子。它们可以显著量存在于烃油中并可在油的中游工艺和运输过程中以及在上游运输中沉淀析出来以及沉积,从而带来不良后果。
业内描述了借助添加剂处理来解决这一问题。例如,US-A-2017/0306215(“′215”)描述了通过在烃中加入有效量的聚酯沥青质分散剂来抑制烃中的沥青质沉淀和/或沉积,所述聚酯沥青质分散剂可通过使每烷基(烯基)的琥珀酸基团平均数小于2.0的烷基(烯基)取代琥珀酸酐与至少一种多元醇反应获得。
发明内容
本发明以与′215不同的方式处理上述问题。使用例如未反应的琥珀酸酐并与金属清净剂组合,其效力在本说明书的实施例部分中证实。
在第一个方面中,本发明提供一种减轻在烃油(如原油)的中游工艺和运输以及上游运输中的,包括储存和调合中的结垢和/或沥青质附聚(或絮凝)的方法,其包括在油中提供一种添加剂组合,该组合包含:
(A)聚烯基取代的羧酸或酐,和
(B)金属清净剂体系,其包含烃基取代的羟基苯甲酸金属盐、或烃基取代的磺酸金属盐或这两种盐的混合物或所述盐的络合物,
其中(A)与(B)的质量:质量比在20:1至1:20,如10:1至1:10,优选3:1至1:3的范围内,且所述添加剂组合的处理率在5、10、100或500至1000、5000或10000,优选100至5000,如500至1000质量ppm的范围内。
在第二个方面中,本发明提供如上文定义的添加剂组合在烃油中用于减轻在油的中游工艺和运输过程中以及在上游运输中的结垢和/或沥青质附聚或絮凝的用途。因此,在任一方面中,结垢和/或沥青质附聚或絮凝可被理解为由经受中游工艺和运输和/或上游运输的烃油(如原油)产生。
具体实施方式
定义
为了举例说明而非限制,提供下列定义。
“下游”是指涉及在炼油厂内或其后的烃油的任何操作,包括精炼产品的运输和利用。
“中游”是指涉及烃油(典型地,原油)从通常位于油田或附近的上游存储输送到炼油厂的任何操作,例如直到并包括在烃油临进入炼油厂之前的储存和管道输送。
“上游”是指涉及通常从油井开采(生产)烃油(典型地,原油)到通常位于油田或附近的储存组件以准备将烃油进一步输送到炼油厂的任何操作。
“原油”是指最初位于地下的烃化石燃料油,将其开采、运输和随后在炼油厂的炼油厂操作中精炼。术语“原油”包括单一类型的原油或含有两种或更多种不同类型的原油的原油掺合物。原油包括中间(轻质)原油、中质原油、重质原油和页岩油;
“烷基”是指不含双键或三键并以支化链或直链排布的一价烃基。
“亚烷基”是指不含双键或三键并以支化链或直链排布的二价烃基。
“烯基”是指含有一个或多个双键并以支化链或直链排布的一价烃基。
“PIB”是指聚异丁烯并包括正常或“常规”聚异丁烯和高反应性聚异丁烯(HRPIB)。
提到某基团是特定聚合物(例如聚丙烯、聚(乙烯-共聚-丙烯)或PIB)时包括了主要含有相应单体以及可忽略量的沿聚合物链的其它取代和/或插入结构的聚合物。换言之,提到某基团是聚丙烯基团时不要求该基团由100%丙烯单体构成而没有任何连接基、取代、杂质或其它取代基(例如亚烷基或亚烯基取代基)。这样的杂质或其它取代基可以相对次要量存在,只要它们与含有100%纯度的相应聚合物取代基(substituent)的相同添加剂相比不影响添加剂的工业性能。
“烃基”是指含有碳和氢原子并经由碳原子键合到该分子的其余部分上的基团或基。其可含有杂原子,即非碳和氢的原子,只要它们不改变该基团的基本烃性质和特征。
如果使用下列词语和措辞,其也具有下文给出的含义:
“活性成分”或“(a.i.)”是指不是稀释剂或溶剂的添加剂材料;
“包含”或任何同源词表明所述要素、步骤或整数或组分的存在,但不排除存在或添加一个或多个其它要素、步骤、整数、组分或其组合;措辞“由...构成”或“基本由...构成”或同源词可涵盖在“包含”或同源词内,其中“基本由...构成”允许包括不会实质影响其适用的组合物的特征的物质;
“主要量”是指组合物的50质量%或更多,优选60质量%或更多,更优选70质量%或更多,再更优选80质量%或更多;
“次要量”是指组合物的少于50质量%,优选少于40质量%,更优选少于30质量%,再更优选少于20质量%;
“TBN”是指如通过ASTM D2896测得的总碱值。
此外,在本说明书中,如果使用的话并且在使用时:
“钙含量”是通过ASTM 4951测得;
“磷含量”是通过ASTM D5185测得;
“硫酸盐灰分含量”是通过ASTM D874测得;
“硫含量”是通过ASTM D2622测得;
“KV100”是指如通过ASTM D445测得的在100℃下的运动粘度。
还要理解的是,所用各种组分(基本的以及最佳的和常规的)可能在配制、储存或使用条件下反应,本发明也提供由于任何这样的反应可获得或已获得的产物。
此外,要理解的是,本文列出的量、范围和比率的任何上限和下限可以独立地组合。
详述
聚烯基取代的羧酸或酐(A)
其可以是一元或多元羧酸,优选二元羧酸。聚烯基优选具有8至400,如12至100个碳原子。
(A)内的示例性酐的通式可被描绘为
其中R1代表C8至C100支化或直链聚烯基。
聚烯基结构部分可具有200至10000,如350至2000,优选500至1000的数均分子量。
用于形成本发明中所用的酐以生成聚烯基结构部分的合适的烃或聚合物包括均聚物、互聚物或较低分子量烃。一类这样的聚合物包括乙烯和/或至少一种具有式H2C=CHR1的C3至C28α-烯烃的聚合物,其中R1是包含1至26个碳原子的直链或支化链烷基,且其中该聚合物含有碳-碳不饱和,优选高度末端乙烯亚基不饱和。优选地,此类聚合物包括乙烯和至少一种上式的α-烯烃的互聚物,其中R1是具有1至18,更优选1至8,再更优选1至2个碳原子的烷基。因此,可用的α-烯烃单体和共聚单体包括例如丙烯、丁烯-1、己烯-1、辛烯-1、4-甲基戊烯-1、癸烯-1、十二烯-1、十三烯-1、十四烯-1、十五烯-1、十六烯-1、十七烯-1、十八烯-1、十九烯-1及其混合物(例如丙烯和丁烯-1的混合物)。此类聚合物的实例是丙烯均聚物、丁烯-1均聚物、乙烯-丙烯共聚物、乙烯-丁烯-1共聚物和丙烯-丁烯共聚物,其中该聚合物含有至少一些末端和/或内部不饱和。优选的聚合物是乙烯和丙烯以及乙烯和丁烯-1的不饱和共聚物。互聚物可含有次要量,例如0.5至5摩尔%的C4至C18非共轭二烯烃共聚单体。但是,该聚合物优选仅包括α-烯烃均聚物、α-烯烃共聚单体的互聚物和乙烯与α-烯烃共聚单体的互聚物。所用聚合物的摩尔乙烯含量优选为0至80,更优选0至60%。当使用丙烯和/或丁烯-1作为与乙烯的共聚单体时,此类共聚物的乙烯含量最优选为15至50%,但可存在更高或更低的乙烯含量。
这些聚合物可通过使α-烯烃单体、或α-烯烃单体的混合物、或包含乙烯和至少一种C3至C28α-烯烃单体的混合物,在包含至少一种茂金属(例如环戊二烯基-过渡金属化合物)和铝氧烷化合物的催化剂体系存在下聚合制备。使用这种方法,可以提供其中95%或更多的聚合物链具有末端乙烯亚基型不饱和的聚合物。表现出末端乙烯亚基不饱和的聚合物链的百分比可通过FTIR能谱分析、滴定或C13 NMR测定。后一类型的互聚物可通过式POLY-C(R1)=CH2表征,其中R1是C1至C26,优选C1至C18,更优选C1至C8,最优选C1至C2烷基(例如甲基或乙基),且其中POLY代表聚合物链。R1烷基的链长取决于选择用于聚合的共聚单体而变。次要量的聚合物链可含有末端乙烯基(ethenyl),即乙烯基(vinyl)不饱和,即POLY-CH=CH2,且一部分聚合物可含有内部单不饱和,例如POLY-CH=CH(R1),其中R1如上文定义。这些末端不饱和互聚物可通过已知的茂金属化学制备并且也可如美国专利Nos.5,498,809;5,663,130;5,705,577;5,814,715;6,022,929和6,030,930中所述制备。
另一类可用的聚合物是通过异丁烯和苯乙烯的阳离子聚合制成的聚合物。这一类型中的常见聚合物包括通过如下聚合获得的聚异丁烯:使具有35至75质量%的丁烯含量和30至60质量%的异丁烯含量的C4炼油厂料流在路易斯酸催化剂(如三氯化铝或三氟化硼)存在下聚合。用于制造聚正丁烯的单体的优选来源是石油原料流,如残油液II(RaffinateII)。这些原料公开在本领域中,如在美国专利No.4,952,739中。聚异丁烯是最优选的骨架,因为其容易由丁烯料流通过阳离子聚合(例如使用AlCl3或BF3催化剂)获得。此类聚异丁烯通常含有沿链布置的每聚合物链一个烯属双键的量的残留不饱和。一个优选实施方案利用由纯异丁烯料流或残油液I料流制成的聚异丁烯来制备含末端乙烯亚基烯烃的反应性异丁烯聚合物。优选地,被称为高反应性聚异丁烯(HR-PIB)的这些聚合物具有至少65%,例如70%,更优选至少80%,最优选至少85%的末端乙烯亚基含量。例如在美国专利No.4,152,499中描述了此类聚合物的制备。HR-PIB是已知的且HR-PIB可以商品名GlissopalTM(来自BASF)和UltravisTM(来自BP-Amoco)购得。
可用的聚异丁烯聚合物通常基于400至3000的烃链。制造聚异丁烯的方法是已知的。聚异丁烯可如下所述通过卤化(例如氯化)、热“烯”反应或通过使用催化剂(例如过氧化物)的自由基接枝进行官能化。
烃或聚合物骨架可以使用上文提到的三种方法的任一种或其任何顺序的组合,选择性地在该聚合物或烃链上的碳-碳不饱和位点处或沿链无规地,用产生羧酸酐的结构部分来官能化。
用于使聚合物烃与不饱和羧酸、酐反应和由这些化合物制备衍生物的方法公开在美国专利Nos.3,087,936;3,172,892;3,215,707;3,231,587;3,272,746;3,275,554;3,381,022;3,442,808;3,565,804;3,912,764;4,110,349;4,234,435;5,777,025;5,891,953;以及EP 0 382 450 B1;CA-1,335,895和GB-A-1,440,219中。聚合物或烃可通过在导致官能结构部分或试剂(即酸酐)主要在碳-碳不饱和(也称为烯键或烯属不饱和)位点处加成到聚合物或烃链上的条件下使该聚合物或烃反应而用羧酸酐结构部分官能化,使用卤素辅助的官能化(例如氯化)法或热“烯”反应进行。
可以通过将不饱和α-烯烃聚合物卤化(例如氯化或溴化)至基于聚合物或烃的重量计1至8,优选3至7质量%氯或溴来实现选择性官能化,通过在60至250,优选110至160,例如120至140℃的温度使氯或溴经过该聚合物0.5至10,优选1至7小时而进行。卤化的聚合物或烃(下文称为骨架)随后与足量的能将所需数量的官能结构部分加成到骨架上的单不饱和反应物,例如单不饱和羧酸反应物在100至250,通常180至235℃下反应0.5至10,例如3至8小时,以使所得产物含有基于每摩尔卤化骨架所需摩尔数的单不饱和羧酸反应物。或者,将骨架和单不饱和羧酸反应物混合并在向该热材料中加入氯的同时加热。
尽管氯化通常有助于提高原料烯烃聚合物与单不饱和官能化反应物的反应性,但这对考虑用于本发明的一些聚合物或烃而言不是必要的,特别是具有高末端键含量和反应性的那些优选聚合物或烃。因此,优选使骨架和单不饱和官能化反应物(羧酸反应物)在升高的温度下接触以引发初始热“烯”反应。烯反应是已知的。
可通过经各种方法沿聚合物链无规连接官能结构部分来将烃或聚合物骨架官能化。例如,该聚合物可以以溶液或固体形式在自由基引发剂存在下用如上所述的单不饱和羧酸反应物接枝。当在溶液中进行时,接枝在100至260,优选120至240℃的高温下进行。自由基引发的接枝优选在含有例如基于初始总油溶液计1至50,优选5至30质量%聚合物的矿物润滑油溶液中实现。
可用的自由基引发剂是过氧化物、氢过氧化物和偶氮化合物,优选是沸点高于100℃并在接枝温度范围内热分解以提供自由基的那些。这些自由基引发剂的代表是偶氮丁腈、2,5-二甲基己-3-烯-2,5-双叔丁基过氧化物和过氧化二枯烯。引发剂在使用时通常以反应混合物溶液重量的0.005至1重量%的量使用。通常,上述单不饱和羧酸反应物材料和自由基引发剂在1.0:1至30:1,优选3:1至6:1的重量比范围内使用。接枝优选在惰性气氛中,如在氮气覆盖下进行。所得接枝聚合物的特征在于具有沿聚合物链无规连接的羧酸(或衍生物)结构部分,要理解的是,一些聚合物链保持未接枝。上述自由基接枝可用于本发明中所用的其它聚合物和烃。
用于将骨架官能化的优选单不饱和反应物包括一元和二元羧酸材料,即酸或酸衍生材料,包括(i)单不饱和的C4至C10二元羧酸,其中(a)羧基是邻位的(即位于相邻碳原子上)和(b)相邻碳原子的至少一个,优选两者是单不饱和的一部分;(ii)(i)的衍生物,如(i)的酐或C1至C5醇衍生的单酯或二酯;(iii)单不饱和的C3至C10一元羧酸,其中碳-碳双键与羧基共轭,即具有结构结构-C=C-CO-;和(iv)(iii)的衍生物,如(iii)的C1至C5醇衍生的单酯或二酯。也可使用单不饱和的羧酸材料(i)-(iv)的混合物。在与骨架反应时,单不饱和羧酸反应物的单不饱和变饱和。因此,例如,马来酸酐变成骨架取代的琥珀酸酐,丙烯酸变成骨架取代的丙酸。此类单不饱和羧酸反应物的实例是富马酸、衣康酸、马来酸、马来酸酐、氯马来酸、氯马来酸酐、丙烯酸、甲基丙烯酸、巴豆酸、肉桂酸和前述的低碳烷基(例如C1至C4烷基)酸酯,例如马来酸甲酯、富马酸乙酯和富马酸甲酯。
为了提供所需官能度,单不饱和羧酸反应物,优选马来酸酐通常以基于聚合物或烃的摩尔计等摩尔量至100,优选5至50质量%过量的量使用。如果需要,可以通过例如汽提(通常在真空下)从最终分散剂产物中除去未反应的过量单不饱和羧酸反应物。
金属清净剂(B)
金属清净剂是基于所谓金属“皂”,即酸性有机化合物的金属盐的添加剂,有时称为表面活性剂。可用的清净剂包括金属的油溶性中性和高碱性水杨酸盐和磺酸盐,所述金属特别是碱金属或碱土金属,例如钠、钾、锂、钙和镁。最常用的金属是钙和镁,两者都可存在于根据本发明的任一方面的船用燃料组合物中使用的清净剂中。可以使用清净剂的组合,无论是高碱性还是中性还是两者。它们通常包含极性头和长疏水尾。包含中和的金属清净剂作为金属碱(例如碳酸盐)胶束外层的高碱性金属清净剂可以通过如下方式提供:使过量金属碱(如氧化物或氢氧化物)与酸性气体(如二氧化碳)反应而含有大量金属碱。
在本发明中,金属清净剂(B)可以是金属烃基取代的羟基苯甲酸盐,更优选烃基取代的水杨酸盐清净剂。该金属可以是碱金属(例如Li、Na、K)或碱土金属(例如Mg、Ca)。
作为烃基的实例,可以提到烷基和烯基。优选的高碱性金属烃基取代的羟基苯甲酸盐是烷基取代的水杨酸钙并具有下示结构:
其中R是直链烷基。苯环上可以连接有多于一个R基团。COO-基团可以在羟基的邻位、间位或对位;邻位是优选的。R基团可以在羟基的邻位、间位或对位。
水杨酸通常通过苯氧化物的羧化、通过Kolbe-Schmitt法制备,在这种情况下通常与未羧化的酚混合获得(通常在稀释剂中)。水杨酸可以是未硫化或硫化的,并且可以化学改性和/或含有附加取代基。硫化烷基水杨酸的方法是本领域技术人员公知的,并描述在例如US 2007/0027057中。
烷基可含有8至100,有利地8至24,如14至20个碳原子。
本发明的磺酸盐可由磺酸制备,所述磺酸通常通过烷基取代的芳烃(如由石油分馏或通过芳烃的烷基化获得的那些)的磺化获得。实例包括通过将苯、甲苯、二甲苯、萘、联苯或它们的卤素衍生物如氯苯、氯甲苯和氯萘烷基化而得的那些。烷基化可在催化剂存在下用具有3至多于70个碳原子的烷基化剂进行。烷芳基磺酸盐通常含有每烷基取代的芳族结构部分9至80个或更多碳原子,优选16至60个碳原子。该油溶性磺酸盐或烷芳基磺酸可用金属的氧化物、氢氧化物、烷氧化基物、碳酸盐、羧酸盐、硫化物、氢硫化物、硝酸盐、硼酸盐和醚中和。考虑最终产物的所需TBN来选择金属化合物的量,但通常为化学计算所需量的100至220质量%(优选至少125质量%)。
术语“高碱性”常用于描述金属结构部分的当量数与酸结构部分的当量数的比率大于1的金属清净剂。术语“低碱性”用于描述金属结构部分与酸结构部分的当量比大于1且最多大约2的金属清净剂。
“表面活性剂的高碱性钙盐”是指其中油不溶性金属盐的金属阳离子基本是钙阳离子的高碱性清净剂。在该油不溶性金属盐中可存在少量的其它阳离子,但该油不溶性金属盐中的通常至少80,更通常至少90,例如至少95摩尔%的阳离子是钙离子。钙以外的阳离子可例如源自在高碱性清净剂的制造中使用其中阳离子是钙以外的金属的表面活性剂盐。表面活性剂的金属盐优选也是钙。
碳酸化的高碱性金属清净剂通常包含非晶纳米粒子。另外,本领域公开了包含结晶方解石和球霰石形式的碳酸盐的纳米微粒材料。
清净剂的碱度可表示为总碱值(TBN),有时称为碱值(BN)。总碱值是中和高碱性材料的所有碱度所需的酸的量。TBN可以使用ASTM标准D2896或等效程序测量。清净剂可具有低TBN(即小于50的TBN)、中TBN(即50至150的TBN)或高TBN(即大于150,如150-500的TBN)。碱度也可表示为碱度指数(BI),其是高碱性清净剂中的总碱与总皂的摩尔比。
本发明的实施方案
中游和上游操作可以根据ISO20815 2018进行。
概括而言,如广泛理解地,中游操作涉及石油工业的加工和运输部门,例如运输管道和终端;上游操作可能涉及原油的运输,作为非限制性实例包括原油开采(production/extracxtion)操作。因此,通常,上游运输和中游加工和运输中的烃油是原油。
在开采操作中,油通常从地下出来运输(流动)到加工/分离单元以除水,然后运输到储存以从油田移走。沥青质沉淀可在立管中或地上发生,例如在来自多个井的油混入储罐时发生。上游运输可包括加工步骤,如水分离、气体分离、固体分离或用于热裂解或催化裂解油的提质器(upgraders)、或在生产现场附近溶剂洗涤油以在运输到炼油厂之前降低粘度,以例如符合中游或炼油厂规范。因此,提质可被视为为后续操作改进原油的性质,因此产生提质的原油而非精炼产物。附加地或替代性地,上游加工步骤可涉及使用其它添加剂,例如用于水分离、气体分离、防止蜡沉积、防止沥青质沉积、防垢和防腐蚀。所有上述加工步骤也可能在中游操作过程中发生。关于它们各自的活动(activities),上游和中游操作都也可包括储存和调合。上游运输通常经由管道发生(尽管可附加地或替代性地包括其它运输方法),而中游加工和运输可能涉及各种运输方法,包括但不限于使用卡车、轨道、船舶(油轮)、驳船和管道,以及在运输步骤与在炼油厂外的进一步储存之间的多个储存位置。
另一方面,下游操作通常被理解为从(临近)精炼活动开始并包括所得精炼产物的后续利用,例如作为润滑剂基础油料、成品润滑剂、石油化学品和燃料,如汽油、柴油或重质燃料油。因此,在一些实施方案中,本公开中的下游工艺从烃油,如原油进入炼油厂、进入炼油工艺或进入炼油厂中的脱盐单元前的加热单元的点开始,而中游工艺和运输以及上游运输在这一点之前发生。本公开中的中游工艺和运输以及上游运输因此可一起在烃油(例如原油)进入或已进入炼油厂或原油烃精炼组件之前发生。本文所用的“原油烃精炼组件”通常是指精炼原油烃的工艺,如炼油工艺的装置或工具。原油烃精炼组件位于炼油厂内,并包括为制造精炼产物而进行的工艺。典型的原油烃精炼组件包括但不限于:传热组件,如热交换器、炉、原油预热器、原油蒸馏塔、减压蒸馏塔、炼焦器预热器、或任何其它加热器、FCC淤浆塔(FCC slurry bottom)、脱丁烷塔交换器/塔、其它进料/流出物交换器,以及在炼油厂设施中的炉空气预热器、在炼油厂设施中的火炬压缩机(flare compressor)组件和在石油化学设施中的蒸汽裂解器/转化炉管。原油烃精炼组件还可包括可发生传热的其它工具,如分馏或蒸馏塔、洗涤塔、反应器、液体夹套管、管式炉(pipestill)、炼焦器和减粘裂化炉。
本发明考虑了可包含添加剂(A)和(B)、由或基本由添加剂(A)和(B)构成的添加剂组合。相应地,尽管本文中提到的添加剂组合的处理率考虑的是活性成分(A)和(B)对烃油(如原油)的总处理率,但要理解的是,该添加剂组合可与溶剂、稀释剂或其它添加剂结合或同时存在于或引入烃油中,所述其它添加剂例如为破乳剂(用于破乳)、缓蚀剂(优选水溶性)、水合物抑制剂、阻垢剂、流动改进剂、蜡沉积抑制剂(或石蜡抑制剂)、倾点下降剂、粘度改进剂和/或其它流体。其它组分如上列那些可以附加地或替代性地与本发明中提到的添加剂组合分开地,例如在该添加剂组合之前或之后添加或与烃油掺合。换言之,在本文中提到添加剂组合由添加剂(A)和(B)构成时不排除通常向烃油如原油中加入其它添加剂,作为非限制性实例包括将该添加剂组合与其它添加剂合并(这可能意味着单独合并添加剂(A)和(B))以形成用于烃油的添加剂套装。
(A)与(B)的质量:质量比可在1:1至1:6,如1:1至1:3的范围内。
在这些比率中可提到:
1(PIBSA):3(水杨酸盐);
1(PIBSA):3(水杨酸盐):3(磺酸盐);
1(PIBSA):2(水杨酸盐):2(磺酸盐);和
1(PIBSA):1(水杨酸盐):1(磺酸盐)。
在(B)中,所述清净剂或各清净剂可具有在下限为0、50、100或150且上限为300、350、400、450或500的范围内的TBN。
在(B)中,所述组分清净剂或各组分清净剂可作为高碱性清净剂存在。
添加剂(A)和(B)可与如下添加剂一起使用或用作如下添加剂:破乳剂(用于破乳)、缓蚀剂(优选水溶性)、水合物抑制剂、阻垢剂、流动改进剂、蜡沉积抑制剂(或石蜡抑制剂)、倾点下降剂、粘度改进剂和/或其它流体。
实施例
下列非限制性实施例例示本发明。
原油
使用下列原油:
原油No. | 硫含量(%wt/wt) |
1 | 3.86 |
2 | 3.9 |
3 | 3.25 |
4 | 0.493 |
5 | 0.012 |
6 | 未测量 |
添加剂组分
使用下列组分:
(A)80%聚异丁烯琥珀酸酐(“PIBSA”)和20%SN150形式的稀释剂(I类油),所述PIBSA衍生自具有950的数均分子量的聚异丁烯,
(B1)具有225的TBN的高碱性水杨酸钙清净剂,
(B2)具有302的TBN的高碱性磺酸钙清净剂。
试验方法
应用下列方法:
原油沥青质稳定性(涵盖“抑制”)
在改良版本的ASTM D7157设备中进行试验并证实原油耐受在加入庚烷时失去稳定的能力。结果被记录为“S”值,油在沥青质沉淀方面的固有稳定性。较高“S”值意味着油在沥青质絮凝方面更稳定。
沥青质分散力
该试验观察沥青质附聚物沉降到容器(管)底部的沉降速率并测量添加剂分散絮凝的沥青质的能力。测试在环境温度和压力下进行并且结果表示为mL/h沉积物。这一程序包括取0.5克沥青质原油,在存在或不存在添加剂的情况下用大约0.5毫升甲苯稀释。加入过量链烷流体(直到100mL),通常是庚烷,并充分摇振该容器。然后让管静置,其中摄像机监测沥青质附聚物/粒子随时间的沉降速率,较低速率值表明优异的结果。
沉积物控制
这一试验测量沉积到加热表面上的沥青质的减少。
该试验使用150毫升不含添加剂(作为对照)和含有1000或500质量ppm如下列结果表中所示的添加剂组分的原油掺合物样品进行,所述添加剂组分作为稀释物(cutback)添加到掺合物中。作为与现有技术的比较,用琥珀酰亚胺添加剂进行试验,该琥珀酰亚胺添加剂包含PIBSA(1000MW)与四亚乙基五胺(42%ai和44KOH/g的碱值)的反应产物(在下列结果表中被称为PIBSAPAM)。
该试验使用旨在模拟炼油厂防垢剂性能的定制台架试验。该台架是具有串联的五个独立加热试验段的仪器。各试验段包含装在钢外壳中的电阻加热的钢棒,钢外壳与棒电隔离。试验原油样品在棒与外壳之间的空腔中流动。控制在棒中心点的棒温度并在试验全程保持恒定。
当原油流过热棒时,其从该棒吸收热;记录离开试验段的燃料的温度。
如果沉积物积聚在棒表面上,它们降低从棒到原油的传热效率,因此导致离开试验段的原油的温度降低。
计算在试验开始与结束之间的原油出口温度差并对所有五个棒合计。较大的数值表明较高的温度差和因此表明较糟糕的结垢。
试验用125、195、235、275和315℃的各棒温度进行6小时;和用120、160、200、240和280℃的各棒温度进行5小时。
结果以沉积物的毫克数表示。
实验程序和结果
使用上述三个试验测试具有或不具有添加剂处理的原油。结果概括在下表中。
看出本发明的实施例1-14整体上表现好于对照并且好于对比例1-3。
Claims (14)
1.一种减轻在原油的中游工艺和运输以及上游运输中的,包括储存和调合中的结垢和/或沥青质附聚(或絮凝)的方法,其包括在原油中提供一种添加剂组合,该组合包含:
(A)聚烯基取代的羧酸或酐,和
(B)金属清净剂体系,其包含烃基取代的羟基苯甲酸金属盐、或烃基取代的磺酸金属盐或这两种盐的混合物或所述盐的络合物,
其中(A)与(B)的质量:质量比在20:1至1:20,如10:1至1:10,优选3:1至1:3的范围内,且所述添加剂组合的处理率在5质量ppm、10质量ppm、100质量ppm或500质量ppm至1000质量ppm、5000质量ppm或10000质量ppm的范围内,优选100至5000质量ppm,如500至1000质量ppm的范围内。
2.权利要求1的方法,其中所述中游和上游操作根据ISO 20815 2018。
3.权利要求1或权利要求2的方法,其中(A)与(B)的质量:质量比在1:1至1:6,如1:1至1:3的范围内。
4.权利要求1至3任一项的方法,其中在(A)中,所述聚烯基取代基具有8至400个碳原子,优选12至100个碳原子,更优选16至64个碳原子。
5.权利要求1至4任一项的方法,其中在(A)中,所述聚烯基取代基具有350至2000,优选500至1000的数均分子量。
6.权利要求1至5任一项的方法,其中(A)是琥珀酸酐。
7.权利要求6的方法,其中(A)是聚异丁烯琥珀酸酐。
8.权利要求1至7任一项的方法,其中在(B)中,所述金属是钙。
9.权利要求1至8任一项的方法,其中在(B)中,所述烃基取代的羟基苯甲酸盐是水杨酸盐。
10.权利要求1至9任一项的方法,其中在(B)中,所述烃基具有8至100个碳原子,如8至24个碳原子,优选14至20个碳原子。
11.权利要求1至10任一项的方法,其中在(B)中,所述清净剂或各清净剂具有在下限为0、50、100或150且上限为300、350、400、450或500的范围内的TBN。
12.权利要求1至11任一项的方法,其中在(B)中,所述清净剂或各清净剂作为高碱性清净剂存在。
13.权利要求1至12任一项的方法,其中添加剂(A)和(B)与如下添加剂一起使用或用作如下添加剂:破乳剂(用于破乳)、缓蚀剂(优选水溶性)、水合物抑制剂、阻垢剂、流动改进剂、蜡沉积抑制剂(或石蜡抑制剂)、倾点下降剂、粘度改进剂和/或其它添加剂。
14.如权利要求1至13任一项中所述的添加剂组合在原油中用于减轻在原油的中游工艺和运输过程中以及在上游运输中的结垢和/或沥青质附聚或絮凝的用途。
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- 2019-12-09 CN CN201911249047.0A patent/CN111349461B/zh active Active
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EP3760696B1 (en) | 2021-10-27 |
SG10201911804SA (en) | 2020-07-29 |
KR20200077415A (ko) | 2020-06-30 |
EP3760696A1 (en) | 2021-01-06 |
US10995287B2 (en) | 2021-05-04 |
CA3064231A1 (en) | 2020-06-20 |
US20200224109A1 (en) | 2020-07-16 |
JP7482623B2 (ja) | 2024-05-14 |
CN111349461B (zh) | 2023-08-29 |
JP2020114912A (ja) | 2020-07-30 |
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