CN101802145A - 由生物可再生原料制造柴油机燃料 - Google Patents
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Abstract
已经开发出由可再生原料(例如植物油和动物油、脂肪以及油脂)制造柴油沸程燃料的方法。该方法包括通过氢化和脱氧(即脱羧、脱羰和/或加氢脱氧)处理可再生原料,以提供可用作柴油沸程燃料或柴油沸程燃料调合组分的烃级分。如果需要,可以将该烃级分异构化以改进冷流性质。选择性地分离一部分氢化和脱氧的原料,并然后再循环到处理区以提高反应混合物的氢溶解度。
Description
背景技术
本发明涉及由可再生原料(例如在如植物油、鱼油、动物脂肪和油脂的材料中存在的甘油三酸酯和游离脂肪酸)制造可用作运输燃料的柴油沸程烃的方法。该方法包括在一个或多个反应器中的氢化、脱羧、脱羰、和/或加氢脱氧和异构化。在进入异构化区之前使用选择性热高压氢汽提器从氢化、脱羧和/或加氢脱氧区流出物中至少除去碳氧化物。
由于对柴油沸程燃料的需求在世界范围内增长,因而日益关注用于制造柴油机燃料和柴油机燃料调合组分的非石油原油来源。一种这样的可再生源被称作生物可再生源。这些可再生源包括但不限于:植物油,例如玉米油、菜籽油、低芥酸菜籽油、豆油和藻油,动物脂肪,例如非食用牛脂、鱼油,以及各种废流,例如黄色和褐色油脂和下水道污泥。这些来源的共同特征在于它们由甘油酯和游离脂肪酸(FFA)构成。这两类化合物都含有具有8至24个碳原子的正构脂族碳链。甘油酯或FFAs中的脂族碳链可以是完全饱和的,或是单不饱和、二不饱和或多不饱和的。
本领域中有报道公开了由油类制造烃。例如,US 4,300,009公开了使用结晶硅铝酸盐沸石将植物油(例如玉米油)转化成烃(例如汽油)和化学品(例如对二甲苯)。US 4,992,605公开了通过加氢处理植物油(例如低芥酸菜籽油或葵花油)来制造柴油沸程烃产品。最后,US 2004/0230085A1公开了通过加氢脱氧然后异构化来处理生物来源的烃成分的方法。
申请人已经开发出一种方法,其包括一个或多个将可再生原料氢化、脱氧和异构化的步骤。通过从异构化区的进料中至少除去二氧化碳来改进异构化催化剂的性能。二氧化碳或其它碳氧化物的存在可能造成异构化催化剂的失活。使用选择性热高压氢汽提器除去二氧化碳。
发明概要
本发明涉及由可再生原料制造富含异链烷烃的柴油沸程产物的加氢转化法,其中该方法包括在反应区中通过在反应条件下将可再生原料氢化和脱氧来处理该原料,以提供包含含正链烷烃的烃级分的第一反应产物。在集成的热高压汽提器中,使用氢作为汽提气体从所述第一反应产物中选择性地除去在第一反应区中作为副产物生成的二氧化碳和水。将经过氢汽提的第一反应产物送入加氢异构化反应区。回收异构化的产物。
附图简述
图1和图2是本发明的一个实施方案的示意图。图1是较简单的示意图,而图2更详细。
发明详述
如上所述,本发明涉及由可再生原料(例如源自植物或动物的可再生原料)制造可用作柴油沸程燃料的烃流的方法。这些原料中的一些被称作生物可再生脂肪和油。术语可再生原料包括除获自石油原油的原料之外的原料。可用于本发明的生物可再生原料包括任何包含甘油酯和游离脂肪酸(FFA)的可再生原料。大部分甘油酯是甘油三酸酯,但也可以存在和加工甘油单酸酯和甘油二酸酯。这些原料的实例包括但不限于,低芥酸菜籽油、玉米油、豆油、菜籽油、大豆油、菜油、妥尔油、葵花油、大麻籽油、橄榄油、亚麻籽油、椰子油、蓖麻油、花生油、棕榈油、芥子油、棉籽油、麻风树油、牛脂、黄色和褐色油脂、猪油、鲸骨脂、乳脂肪(fats in milk)、鱼油、藻油、下水道污泥等等。可再生原料的另一些实例包括来自麻风树(Jatropha curcas)(Ratanjoy,野生蓖麻,Jangli Erandi)、Madhuca indica(Mohuwa)、Pongamia pinnata(Karanji Honge)和Azadiracta indicia(印度楝)的非食用植物油。典型的植物或动物脂肪的甘油三酸酯和FFAs在它们的结构中含有具有8至24个碳原子的脂族烃链,大多数该脂肪和油含有高浓度的具有16和18个碳原子的脂肪酸。也可以使用可再生原料和石油衍生烃的混合物或共进料作为原料。可用的、尤其是与上面列举的原料联合作为共进料组分的其它原料组分包括废机油和工业润滑剂,用过的石蜡,由煤、生物质或天然气的气化继之以下游液化步骤(例如费-托技术)而衍生的液体,由废塑料(例如聚丙烯、高密度聚乙烯和低密度聚乙烯)的热解聚或化学解聚而衍生的液体;以及作为石化和化学工艺的副产物生成的其它合成油。也可以使用上述原料的混合物作为共进料组分。在一些用途中,使用共进料组分的一个优点是将来自石油基工艺或其它工艺的被视为废产物的材料转化成当前工艺的有价值的共进料组分。
可用于本发明的可再生原料可以含有多种杂质。例如,妥尔油是木材加工业的副产物,妥尔油除FFAs之外还含有酯和松香酸。松香酸是环羧酸。可再生原料还可能含有污染物,例如碱金属(例如钠和钾)、磷以及固体、水和洗涤剂。任选的第一步骤是尽可能多地除去这些污染物。一种可行的预处理步骤包括在预处理区中在预处理条件下使该可再生原料与离子交换树脂接触。该离子交换树脂是酸性离子交换树脂,例如AmberlystTM-15,并可用作反应器中的床,原料以上行流或下行流方式流过该床。
除去污染物的另一可行手段是温和酸洗。这通过在反应器中使该原料与酸(例如硫酸、硝酸或盐酸)接触来进行。该酸和原料可以在分批法或连续法中接触。通常在环境温度和大气压下用稀酸溶液进行接触。如果以连续方式进行接触,其通常以对流方式进行。从原料中除去金属污染物的又一可行手段是通过使用本领域公知的保护床。这些可以包括具有或不具有脱金属催化剂(例如镍或钴)的氧化铝保护床。过滤和溶剂萃取技术是可用的其它选择。如USAN 11/770,826中所述的加氢处理是可用的另一预处理技术。
该可再生原料流向在一个或多个反应器中包含一个或多个催化剂床的第一反应区。术语“原料”包括未经除污染物处理的原料以及在预处理区中净化过的那些原料。在第一反应区中,使该可再生原料在氢化条件下、在氢存在下与氢化或加氢处理催化剂接触,以使反应性组分(例如所述正链烷烃链的烯属或不饱和部分)氢化。氢化或加氢处理催化剂是本领域公知的任何这样的催化剂,例如分散在高表面积载体上的镍或镍/钼。其它氢化催化剂包括分散在高表面积载体上的一种或多种贵金属催化元素。贵金属的非限制性实例包括分散在γ-氧化铝或活性炭上的Pt和/或Pd。氢化条件包括40℃至400℃的温度和689kPa绝对压力(100psia)至13,790kPa绝对压力(2000psia)的压力。在另一实施方案中,氢化条件包括200℃至300℃的温度和1379kPa绝对压力(200psia)至4826kPa绝对压力(700psia)的压力。该氢化区的其它运行条件是本领域公知的。
上文列举的催化剂也能催化原料的脱羧、脱羰和/或加氢脱氧以除去氧。脱羧、脱羰和加氢脱氧在本文中统称为脱氧反应。脱羧条件包括689kPa(100psia)至6895kPa(1000psia)的较低压力、200℃至400℃的温度和0.5至10hr-1的液时空速。在另一实施方案中,脱羧条件包括689kPa(100psia)至6895kPa(1000psia)的相同的相对低压、288℃至345℃的温度和1至4hr-1的液时空速。由于氢化是放热反应,因此,当原料流经催化剂床时温度升高,并开始发生脱羧和加氢脱氧。因此,可以想到所有反应在一个反应器中或在一个床中同时发生,并在本发明的范围内。或者,可以控制条件,以便在一个床中主要发生氢化,在第二个床中发生脱羧和/或加氢脱氧。当然,如果仅使用一个床,则氢化主要发生在床的前部,而脱羧/加氢脱氧主要发生在该床的中部和底部。最后,所需氢化可以在一个反应器中进行,脱羧、脱羰和/或加氢脱氧可以在独立的反应器中进行。
出自脱氧反应的反应产物包含液态部分和气态部分。液态部分包含烃级分,该烃级分基本全是正链烷烃,并具有高浓度的在9至18个碳原子范围内的链烷烃。气态部分包含氢、二氧化碳、一氧化碳、水蒸气、丙烷,并可能包含硫组分(例如硫化氢)或磷组分(例如膦)。将来自脱氧反应器的流出物导向热高压氢汽提器。热高压氢汽提器的一个目的是将该流出物的至少一部分气态部分与该流出物的液态部分选择性地分离。由于氢是昂贵的资源,为了节省成本,将分离的氢再循环到含有脱氧反应器的第一反应区。此外,如果未从流出物中除去水、一氧化碳和二氧化碳,可能造成异构化区中差的催化剂性能。在热高压氢汽提器中使用氢选择性地汽提水、一氧化碳、二氧化碳、任何氨或硫化氢。用于汽提的氢可以是干燥的,并且不含碳氧化物。温度可以控制在限定范围内以实现所需分离,压力可以保持在与两个反应区大致相同的压力下,以使投资和运行成本最小化。热高压氢汽提器可以在689kPa绝对压力(100psia)至13,790kPa绝对压力(2000psia)的压力和40℃至350℃的温度的条件下运行。在另一实施方案中,热高压氢汽提器可以在1379kPa绝对压力(200psia)至4826kPa绝对压力(700psia)或2413kPa绝对压力(350psia)至4882kPa绝对压力(650psia)的压力和50℃至350℃的温度的条件下运行。热高压氢汽提器可以在与反应区基本相同的压力下运行。“基本”是指热高压氢汽提器的运行压力在反应区运行压力的1034kPa绝对压力(150psia)之内。例如,在一个实施方案中,热高压氢汽提器分离区比反应区低最多1034kPa绝对压力(150psia)。
流出物进入热高压汽提器,至少一部分气态组分被氢汽提气携带,并被分离到塔顶流中。脱氧区流出物流的其余部分作为热高压氢汽提器塔底流被移走,并含有具有例如含8至24个碳原子的直链烃之类的组分的液体烃级分。不同原料会产生不同的链烷烃分布。热高压氢汽提器塔底流中的一部分这种液体烃级分可用作下述烃再循环物。
氢是上述至少一些反应中的反应物,必须溶解足量的氢以最有效地参与催化反应。过去的方法在高压下运行,以使所需量的氢溶解并容易供反应使用。但是,与它们的较低压力对应方法相比,较高压力的操作在建设和运行上成本较高。本发明的一个优点在于工作压力可以为1379kPa绝对压力(200psia)至4826kPa绝对压力(700psia),其低于其它早先操作中的压力。在另一实施方案中,工作压力为2413kPa绝对压力(350psia)至4481kPa绝对压力(650psia),在再一实施方案中,工作压力为2758kPa绝对压力(400psia)至4137kPa绝对压力(600psia)。此外,反应速率提高,以致在给定期间内通过反应器的材料吞吐量更大。可以从工艺流出物中分离氢并再循环到氢化和脱氧区,或氢的量可以仅稍超过氢化和脱氧反应的氢需求量,例如过量5至25%,并因此不循环。可以使用另一精制单元(例如加氢裂化器)作为氢源,其可能消除对循环气体压缩机的需要。
在一个实施方案中,使大量烃再循环到脱氧反应区,从而在较低压力下使所需量的氢保持溶解。其它方法利用烃再循环控制反应区内的温度,因为该反应是放热反应。但是,此处所用的再循环物与原料的比率的范围不取决于温度控制要求,而是取决于氢溶解度要求。氢在烃产物中的溶解度高于其在原料中的溶解度。通过采用大的烃再循环量,大大提高了反应区中氢在整个液相中的溶解度,并且无需较高压力来提高溶解的氢的量。在本发明的一个实施方案中,烃再循环物与原料的体积比为2∶1至8∶1,或2∶1至6∶1。在另一实施方案中,该比率为3∶1至6∶1,在再一实施方案中,该比率为4∶1至5∶1。
尽管在热高压氢汽提器中分离的烃级分可用作柴油沸程燃料,但因为其基本包含正链烷烃,因而具有差的冷流性质。如果需要改进该液体烃级分的冷流性质,可以使该烃级分与异构化催化剂在异构化条件下接触以将正链烷烃至少部分异构化成支链烷烃。第二反应区(异构化区)的流出物是富含支链烷烃的料流。术语“富含”是指该流出物流的支链烷烃浓度高于进入该异构化区的料流,并优选包含多于50质量%支链烷烃。异构化区流出物预计可以含有70、80或90质量%支链烷烃。异构化可以在上述相同反应区(即相同反应器)的独立的床中进行,或异构化可以在独立的反应器中进行。为易于描述,下面针对使用第二反应器进行异构化反应的实施方案。使经过氢汽提的脱氧反应区产物在异构化条件下在氢存在下与异构化催化剂接触,以将正链烷烃异构化成支链烷烃。只需要足以克服正链烷烃的冷流问题的最低支化。由于尝试显著支化具有产生高程度的不想要的裂化的危险,因此主要异构化产物是单支链烃。
链烷烃产物的异构化可以以本领域已知的任何方式或使用本领域已知的任何合适的催化剂实现。可以使用一个或多个催化剂床。异构化优选以并流运行模式运行。固定床、喷淋床下行流或固定床液体填充上行流模式都是合适的。参见例如US 2004/0230085,其全文经此引用并入本文。合适的催化剂包含周期表第VIII族(IUPAC 8-10)的金属和载体材料。合适的第VIII族金属包括铂和钯,它们各自可以独自使用或联合使用。载体材料可以是非晶或结晶的。合适的载体材料包括非晶氧化铝、非晶二氧化硅-氧化铝、镁碱沸石、ALPO-31、SAPO-11、SAPO-31、SAPO-37、SAPO-41、SM-3、MgAPSO-31、FU-9、NU-10、NU-23、ZSM-12、ZSM-22、ZSM-23、ZSM-35、ZSM-48、ZSM-50、ZSM-57、MeAPO-11、MeAPO-31、MeAPO-41、MeAPSO-11、MeAPSO-31、MeAPSO-41、MeAPSO-46、ELAPO-11、ELAPO-31、ELAPO-41、ELAPSO-11、ELAPSO-31、ELAPSO-41、浊沸石、钙霞石、钾沸石、stiubite的氢形式、丝光沸石的镁或钙形式、和帕水硅铝钙石(partheite)的镁或钙形式,它们各自可以独立使用或联合使用。ALPO-31描述在US 4,310,440中。SAPO-11、SAPO-31、SAPO-37和SAPO-41描述在US 4,440,871中。SM-3描述在US 4,943,424;US 5,087,347;US 5,158,665;和US 5,208,005中。MgAPSO是一种MeAPSO,这是金属铝硅磷酸盐分子筛的首字母缩略词,其中金属Me是镁(Mg)。合适的MeAPSO-31催化剂包括MgAPSO-31。MeAPSOs描述在US 4,793,984中,且MgAPSOs描述在US 4,758,419中。MgAPSO-31是优选的MgAPSO,其中31是指具有结构类型31的MgAPSO。具有最初降低的孔径的许多天然沸石,例如镁碱沸石,可以如US 4,795,623和US 4,924,027中教导的那样通过经铵离子交换除去缔合的碱金属或碱土金属、并煅烧产生基本氢形式来转化成适用于烯烃骨架异构化的形式。在US 5,510,306、US 5,082,956和US 5,741,759中公开了用于骨架异构化的其它催化剂和条件。
该异构化催化剂还可以包含如US 5,716,897和US 5,851,949中所述的选自由镧、铈、镨、钕、钐、钆、铽及其混合物组成的组的改性剂。其它合适的载体材料包括ZSM-22、ZSM-23和ZSM-35,它们在US 5,246,566和S.J.Miller著的题为“New molecular sieve process for lube dewaxing bywax isomerization(通过蜡异构化将润滑油脱蜡用的新型分子筛法)”的文章,Microporous Materials 2(1994)439-449中被描述用于脱蜡。US4,310,440;US 4,440,871;US 4,793,984;US 4,758,419;US 4,943,424;US5,087,347;US 5,158,665;US 5,208,005;US 5,246,566;US 5,716,897;和US 5,851,949的教导经此引用并入本文。
US 5,444,032和US 5,608,968教导了由非晶二氧化硅-氧化铝凝胶和一种或多种属于第VIIIA族的金属构成的合适的双官能催化剂,其在含有多于15个碳原子的长链正链烷烃的加氢异构化中有效。也可以使用活性炭催化剂载体。US 5,981,419和US 5,908,134教导了合适的双官能催化剂,其包含:(a)与β-沸石同结构的多孔结晶材料,选自硼硅酸盐(BOR-B)和硼-铝-硅酸盐(Al-BOR-B),其中摩尔比SiO2∶Al2O3高于300∶1;(b)一种或多种属于第VIIIA族的金属,选自铂和钯,其量在0.05至5重量%的范围内。Article V.Calemma等人,App.Catal.A:Gen.,190(2000),207教导了另一合适的催化剂。
异构化催化剂可以是本领域公知的任何这样的催化剂,例如上文描述和列举的那些。异构化条件包括150℃至360℃的温度和1724kPa绝对压力(250psia)至4726kPa绝对压力(700psia)的压力。在另一实施方案中,异构化条件包括300℃至360℃的温度和3102kPa绝对压力(450psia)至3792kPa绝对压力(550psia)的压力。异构化区的其它运行条件是本领域公知的。低压运行允许不借助补充压缩机从另一装置(例如氢装置)任选送入氢,这可以是减少或消除氢再循环的一种选择。当不将氢循环时,送入异构化区的氢量仅稍高于消耗量,超出消耗需求量的5至25%。
然后通过一个或多个分离步骤加工最终流出物流,即在已实施所有反应后获得的料流,以获得可用作柴油机燃料的纯化的烃流。由于最终流出物流既包含液态组分又包含气态组分(它们的不同部分要再循环),因此可以使用多个分离步骤。例如,可以首先在异构化流出物分离器中分离氢,分离出的氢在塔顶流中除去。异构化流出物分离器的合适运行条件包括,例如,230℃的温度和4100kPa绝对压力(600psia)。如果存在低浓度的碳氧化物,或除去碳氧化物,可以将氢再循环回热高压氢汽提器,以既充当汽提气又与残余物合并为塔底流。所述残余物被送往异构化反应区,这样,氢成为异构化反应区进料流的组分,为反应器提供必需的氢分压。氢也是脱氧反应器中的反应物,且不同原料消耗不同量的氢。异构化流出物分离器具有灵活性,以使该方法即使在第一反应区中消耗更大量的氢时也能运行。此外,可以将异构化流出物分离器的残余物或塔底流的至少一部分再循环至异构化反应区,以提高异构化程度。
除去氢后,最终流出物的残余物仍具有液态和气态组分,通过例如空气冷却或水冷之类的技术将其冷却,并送往冷分离器,在此将液态组分与气态组分分离。冷分离器的合适工作条件包括,例如20至60℃的温度和3850kPa绝对压力(560psia)。还分离水副产物流。在冷却和与气态组分分离后,可以将至少一部分液态组分再循环回异构化区,以提高异构化程度。在进入冷分离器之前,可以将最终流出物流的残余物与热高压氢汽提器塔顶流合并,并且可以将所得合并流送入冷分离器。
液态组分含有可用作柴油机燃料的烃,被称作柴油沸程烃,以及少量的石脑油和LPG。分离的液态组分可以作为柴油机燃料回收,或其可以在产物汽提器中进一步提纯,该产物汽提器将较低沸点的组分和溶解的气体与含C8至C24直链和支链烷烃的柴油产物分离,分离成LPG和石脑油流。产物汽提器的合适运行条件包括20至200℃的塔顶温度和0至1379kPa绝对压力(0至200psia)。
可以在脱丁烷塔或脱丙烷塔中进一步分离LPG和石脑油流,以将LPG分离到塔顶流中,将石脑油留在塔底流中。这种单元的合适工作条件包括20至200℃的塔顶温度和0至2758kPa绝对压力(0至400psia)。LPG可以作为有价值的产品出售或可用在其它工艺中,例如加入氢制造设施中。类似地,石脑油可用在其它工艺中,例如加入氢制造设施中、共同加入重整工艺中,或可用作例如汽油调合组合物(blending pool)中的燃料调合组分。
在产物分离器中分离的气态组分主要包含来自脱羧反应的氢和二氧化碳。也可能存在其它组分,例如一氧化碳、丙烷和硫化氢或其它含硫组分。最好使氢再循环至异构化区,但如果不除去二氧化碳,其浓度会迅速累积并影响异构化区的运行。可以通过本领域公知的手段,例如与热碳酸盐溶液反应、变压吸收等,从氢中除去二氧化碳。也可以如经此引用并入本文的共同待审的申请Docket No.H0013966和Docket No.H0017132中所教导使用胺吸收剂。如果需要,可以通过再生废吸收介质来回收基本纯的二氧化碳。
类似地,可能存在含硫组分,例如硫化氢,以保持脱氧催化剂的硫化物状态或控制脱羧反应与氢化反应(这二者都发生在脱氧区中)的相对量。通常控制硫的量,因此必须在将氢再循环之前除去硫。可以使用例如用胺吸收的技术或通过碱洗除去硫组分。当然,根据所用技术,例如氢选择性膜,可以在单个分离步骤中除去二氧化碳和含硫组分以及其它组分。
可以将除去至少二氧化碳后留下的氢再循环至反应区(在此主要发生氢化)和/或任何后继床/反应器。可以将再循环流送入反应区和/或任何后继床或反应器的入口。烃再循环的一个益处是控制各个床内的温度升高。但是,如上所述,烃再循环量可能取决于反应区中的所需氢溶解度,其超过用于温度控制的量。提高氢在反应混合物中的溶解度就可以在较低压力和因此较低成本下成功运行。
列出下列实施方案以举例说明本发明,但不是要不适当地限制如所附权利要求所述的本发明的宽范围。首先参照图1概括描述该方法,然后参照图2更详细描述该方法。
如图1所示,可再生原料102与再循环氢126一起进入脱氧反应区104。在热高压氢汽提器108中使用氢114a将脱氧产物106汽提。用氢在塔顶流110中除去碳氧化物和水蒸汽。将经过选择性汽提的脱氧产物与再循环氢126a和补充氢114b一起送往异构化区116。将异构化产物118与塔顶流110合并并送往产物回收区120。从产物回收区120中除去碳氧化物流128、轻馏分流130、水副产物流124、烃流126和富含支链烷烃的产物122。可收集富含支链烷烃的产物122用作柴油机燃料,且将氢流126再循环至脱氧反应区104。
如图2所示,该方法以可再生原料流2开始,再生原料流2可经过任选的进料缓冲罐。将该原料流与再循环气流68和再循环流16合并,形成合并的进料流20,将其与反应器流出物热交换,然后送入脱氧反应器4。可以在将再循环物与进料合并之前或之后进行该热交换。脱氧反应器4可含有图2中标示为4a、4b和4c的多个床。脱氧反应器4含有至少一种能够催化原料的脱羧和/或加氢脱氧以除去氧的催化剂。从脱氧反应器4中移出含有脱羧和/或加氢脱氧产物的脱氧反应器流出物流6,并使其与含有脱氧反应器进料的料流20热交换。料流6包含液态组分和气态组分,液态组分主要含有柴油沸程正链烷烃,气态组分主要含有氢、气态水、一氧化碳、二氧化碳和丙烷。
然后将脱氧反应器流出物流6送往热高压氢汽提器8。管道10中的补充氢被分成两部分,料流10a和10b。料流10a中的补充氢也被送入热高压氢汽提器8。在热高压氢汽提器8中,使用补充氢10a和再循环氢28从脱氧反应器流出物6的液态组分中选择性汽提脱氧反应器流出物6的气态组分。将包含氢、气态水、一氧化碳、二氧化碳和至少一部分丙烷的溶解的气态组分选择性地分离到热高压氢汽提器塔顶流14中。脱氧反应器流出物6的残余液态组分(主要包含辛烷值为60至100的具有8至24个碳原子的正链烷烃)作为热高压氢汽提器塔底流12移出。
一部分热高压氢汽提器塔底流形成再循环流16,将其与可再生原料流2合并,产生合并的进料20。可以将另一部分再循环流16,任选料流16a,直接送往脱氧反应器4,并在级间位置(例如床4a和4b之间和/或床4b和4c之间)加入,以例如有助于温度控制。在料流12中的其余热高压氢汽提器塔底流与氢流10b合并以形成合并流18,将其送往异构化反应器22。料流18可以与异构化反应器流出物24热交换。
在管道24中将含有氢和丙烷气态部分以及富含支链烷烃的液态部分的异构化反应器产物取出,并在任选与料流18热交换后,送入氢分离器26。来自氢分离器26的塔顶流28主要含有氢,可以将其再循环回热高压氢汽提器8。使用空气冷却器32将来自氢分离器26的塔底流30空气冷却,并送入产物分离器34。在产物分离器34中,将包含氢、一氧化碳、硫化氢、二氧化碳和丙烷的料流气态部分在料流36中取出,而将该料流的液体烃部分在料流38中取出。也可以从产物分离器34中除去水副产物流40。将料流38送入产物汽提器42,在此将具有较高相对挥发性的组分分离到料流44中,经由管道46从产物汽提器42中提取残余物柴油沸程组分。将料流44送入分馏塔48,分馏塔48用于将LPG分离到塔顶流50中,留下石脑油塔底流52。可以使用任何任选的管道72、74或76,以将至少一部分异构化区流出物再循环回异构化区,提高异构化成支链烷烃的正链烷烃的量。
来自产物分离器34的蒸气流36含有异构化流出物的气态部分,其至少包含氢、一氧化碳、硫化氢、二氧化碳和丙烷,将其送往胺吸收器系统以从蒸气流中分离二氧化碳和硫化氢。由于氢的成本,最好将氢再循环至脱氧反应器4,但使二氧化碳或过量的含硫组分循环是不合意的。为了将含硫组分和二氧化碳与氢分离,使蒸气流36通过由至少两个胺吸收器(也称作涤气器)构成的系统,其以第一胺吸收区56为开始。选用在第一胺涤气器56中的胺能够选择性除去至少这两种相关组分——二氧化碳和硫组分,例如硫化氢。合适的胺可获自DOW和获自BASF,在一个实施方案中,该胺是被促进或活化的甲基二乙醇胺(MDEA)。参见US 6,337,059,其全文经此引用并入本文。来自DOW的适用于第一胺吸收区的胺包括UCARSOLTM AP系列溶剂,例如AP802、AP804、AP806、AP810和AP814。二氧化碳和硫化氢被胺吸收,而氢通过第一胺涤气区并进入管道68以再循环至第一反应区。使胺再生,并释放二氧化碳和硫化氢,并在管道62中除去。在第一胺吸收区中,再生的胺可以循环再利用。释放的二氧化碳和硫化氢在管道62中被送往第二胺涤气区58,其含有对硫化氢选择性但对二氧化碳非选择性的胺。合适的胺仍可获自DOW和获自BASF,在一个实施方案中,该胺是被促进或活化的MDEA。来自DOW的适用于第二胺吸收区的胺包括UCARSOLTM HS系列溶剂,例如HS101、HS102、HS103、HS104、HS115。因此,二氧化碳通过第二胺涤气区58并进入管道66。可以使胺再生,其将硫化氢释放到管道60中。再生的胺然后被再利用,且可将硫化氢再循环至脱氧反应区。第一涤气区的条件包括30至60℃的温度。第一吸收器基本在与反应区相同的压力下运行。“基本”是指该第一吸收器的运行压力在反应区运行压力的1034kPa绝对压力(150psia)内。例如,第一吸收器的压力比反应区的低最多1034kPa绝对压力(150psia)。第二胺吸收区在138kPa绝对压力(20psia)至241kPa绝对压力(35psia)的压力范围内。此外,至少第一吸收器在比分离器高至少1℃的温度运行。使吸收器保持比分离器热有助于使任何轻质烃保持气相,并防止轻质烃冷凝到吸收剂溶剂中。
Claims (10)
1.由可再生原料制造富含支链烷烃的柴油沸程烃产物的方法,包括:
a)在第一反应区中通过使用催化剂在反应条件下在氢存在下将原料氢化和脱氧而处理该原料,以提供第一反应区产物流,所述第一反应区产物流包含氢、二氧化碳和含柴油沸程正链烷烃的烃级分;和
b)在热高压氢汽提器中从所述第一反应区产物流中选择性地分离包含至少一部分氢、水和碳氧化物的气态流,并将至少包含正链烷烃的残余物流送入第二反应区以在异构化条件下接触异构化催化剂,从而将至少一部分正链烷烃异构化并产生富含支链烷烃的料流。
2.权利要求1的方法,进一步包括:
c)将所述富含支链烷烃的料流与所述气态流合并,以形成合并流;
d)将所述合并流冷却,并将至少包含氢和二氧化碳的气态组分与液体烃组分和水组分分离;和
e)回收所述液体烃组分。
3.权利要求1的方法,进一步包括从所述富含支链烷烃的料流中除去至少一部分氢,并将从所述富含支链烷烃的料流中除去的氢再循环至热高压氢汽提器。
4.权利要求2的方法,进一步包括将所述至少包含氢和二氧化碳的气态组分再循环至第一反应区,将所述液体烃组分分离成LPG和石脑油流以及柴油沸程流,将所述LPG和石脑油流分离成LPG流和石脑油流,并将至少一部分石脑油流再循环至第二反应区。
5.权利要求1的方法,进一步包括将一部分所述至少包含正链烷烃的残余物流再循环至第一反应区,再循环物与原料的体积比为2∶1至8∶1。
6.权利要求1的方法,其中第一反应区中的反应条件包括40℃至400℃的温度和689kPa绝对压力(100psia)至13,790kPa绝对压力(2000psia)的压力,且其中所述热高压氢汽提器在第一反应区的1034kPa绝对压力(150psia)内的压力下运行。
7.权利要求1的方法,进一步包括将至少一部分富含支链烷烃的料流再循环至第二反应区。
8.权利要求4的方法,进一步包括在将所述气态组分再循环至第一反应区之前从该气态组分流中分离二氧化碳,和在将所述气态组分再循环至第一反应区之前从该气态组分流中分离含硫组分。
9.权利要求1的方法,其中第二反应区在比第一反应区的压力高至少345kPa绝对压力(50psia)的压力下运行。
10.权利要求1的方法,其中所述可再生原料选自由下述材料组成的组:低芥酸菜籽油、玉米油、豆油、菜籽油、大豆油、菜油、妥尔油、葵花油、大麻籽油、橄榄油、亚麻籽油、椰子油、蓖麻油、花生油、棕榈油、芥子油、棉籽油、麻风树油、牛脂、黄色和褐色油脂、猪油、鲸骨脂、乳脂肪、鱼油、藻油、下水道污泥、ratanjoy油、野生蓖麻油、jangli油、erandi油、mohuwa油、karanji honge油、印度楝树油及其混合物,并可以任选包含至少一种选自由下述材料组成的组的共进料:石油衍生的烃、废机油、废工业润滑剂、用过的石蜡、由煤的气化继之以下游液化步骤而衍生的液体、由生物质的气化继之以下游液化步骤而衍生的液体、由天然气的气化继之以下游液化步骤而衍生的液体、由废塑料的热解聚或化学解聚而衍生的液体、和作为石化工艺和化学工艺的副产物生成的合成油。
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CN104661988A (zh) * | 2012-09-20 | 2015-05-27 | 纳幕尔杜邦公司 | 使用可再生的原料制备直链的长链烷烃的方法 |
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Also Published As
Publication number | Publication date |
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EP2190955A4 (en) | 2011-01-05 |
TWI390030B (zh) | 2013-03-21 |
EP2190955A1 (en) | 2010-06-02 |
WO2009038965A1 (en) | 2009-03-26 |
US7999142B2 (en) | 2011-08-16 |
TW200920834A (en) | 2009-05-16 |
PE20090923A1 (es) | 2009-07-18 |
CL2008002755A1 (es) | 2009-07-31 |
US20090077866A1 (en) | 2009-03-26 |
AR068490A1 (es) | 2009-11-18 |
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