CN112912471A - 联合生产航空燃料和柴油的方法 - Google Patents
联合生产航空燃料和柴油的方法 Download PDFInfo
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- CN112912471A CN112912471A CN201980069855.0A CN201980069855A CN112912471A CN 112912471 A CN112912471 A CN 112912471A CN 201980069855 A CN201980069855 A CN 201980069855A CN 112912471 A CN112912471 A CN 112912471A
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- Prior art keywords
- fraction
- feedstock
- isomerization
- hydrocracking
- product
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Abstract
本公开涉及一种用于从作为可再生原料或含氧化合物原料的原料生产适合用作喷气燃料的烃馏分的工艺设备和方法,其包括以下步骤:将原料与一定量的经加氢裂化的中间产物和任选的另外的液体稀释剂组合,以形成组合的原料;引导所述组合的原料与在加氢处理条件下在加氢脱氧中具有催化活性的材料接触,以提供经加氢脱氧的中间产物;将所述经加氢脱氧的中间产物分离成至少两个馏分:蒸汽馏分和液体馏分;任选地提供一定量的所述液体馏分作为所述液体稀释剂;引导至少一定量的所述液体馏分与在异构化条件下在异构化中具有催化活性的材料接触,以提供经异构化的中间产物;使所述经异构化的中间产物分馏,以提供至少适合用作喷气燃料的烃和底部馏分;引导至少一定量的所述底部馏分与在加氢裂化条件下在加氢裂化中具有催化活性的材料接触,以提供经加氢裂化的中间产物,其相关的益处是,所述方法非常适合于将较高沸点的可再生原料有效地转化为较低沸点的产物,例如非化石煤油。除了所述喷气燃料之外,还可以生产柴油和其他烃。
Description
迄今为止,含氧化合物(如可再生物)在加氢处理中的转化一直集中在制造柴油上,因为石蜡对应于生物材料的典型脂肪酸,例如植物油和动物脂肪(C14、C16和C18),其通常的沸点为250℃至320℃,与通常的沸点为150℃至380℃的柴油产品很好地相对应。喷气燃料(jet fuel)产品要求的沸点范围为120℃至300℃,这意味着需要将来自可再生原料的石蜡的一定量的重质部分转化为更轻质的材料,以仅生产喷气燃料。本公开涉及通过选择性地将重质材料转化为更轻质的材料而具有满足通常产品要求的液体运输燃料(特别是可再生柴油和可再生喷气燃料)的混合物的高产率的方法。
在设计用于制造柴油的单元中对可再生原料进行加氢处理期间,经常还会产生一定量的喷气燃料。但是,人们的兴趣在于将主要在柴油范围内沸腾的可再生原料的中间产物灵活且良好受控地转化为喷气燃料产物,这需要大量转化。
控制源自加氢处理的酯和脂肪酸的喷气燃料的质量的标准是ASTM D7566,A2.1,其中特别规定了沸点曲线和组成。这些性质中的大多数都可以通过加氢处理和分馏而轻松实现。但是,要特别注意满足最高-40℃的凝固点(FP)要求以及最大为0.5wt/wt%的总芳族化合物含量。此外,该标准通过要求T10(即低于该温度,10%发生沸腾)为205℃以下而要求一定量的低沸点产品。根据ASTM D86,将最终沸点(FBP)规定为300℃,这意味着需要将所有沸点为300℃以上的物质转化为更轻质的组分,以落入喷气燃料范围。
现在,根据本公开,提出以逆相两阶段设置进行柴油和喷气燃料的联合生产,其中进料在第一阶段被加氢脱氧,并且在除去酸性气体之后将产物异构化,并可能进行加氢脱芳构化,最后进行分馏。产物的重质馏分在加氢脱氧催化剂的上游再循环,以通过加氢裂化催化剂转化。通过这种方法,加氢裂化可以在第一阶段用较便宜的基础金属催化剂或者较特异性且昂贵的贵金属催化剂进行,而异构化可以在选择性的贵金属催化剂上进行,从而导致特定的凝固点降低。如果芳族化合物的量太高,则可以优化异构化条件以同时去除芳族化合物,或者为此目的可以提供特定的催化剂。
在下文中,术语“阶段”应当用于方法中不进行任何分离的工段。
在下文中,缩写ppmw应当用于表示每百万份重量的份数,即mg/kg。
在下文中,缩写ppm摩尔应当用于表示每百万份的原子份数。
在下文中,缩写ppmv应当用于表示每百万份的体积份数,例如摩尔气体浓度。
在下文中,缩写wt/wt%应当用于表示重量百分比。
在下文中,缩写vol/vol%应当用于表示气体的体积百分比。
在下文中,术语“可再生原料或烃”应当用于表示源自生物来源或废物再循环的原料或烃。化石来源的再循环的废物,例如塑料,也应被视为可再生的。
在下文中,术语“加氢脱氧”应当用于表示在氢的存在下通过形成水而从含氧化合物中除去氧,以及在氢的存在下通过形成碳氧化物而从含氧化合物中除去氧。
在下文中,术语“分子筛的拓扑结构”以“Atlas of Zeolite Framework Types”,第六修订版,Elsevier,2007中描述的含义使用,并且据此使用三个字母的骨架类型代码。
本公开的广泛方面涉及一种用于由含氧化合物原料生产适合用作喷气燃料的烃馏分的方法,该方法包括以下步骤:将原料与一定量的经加氢裂化的中间产物和任选的另外的液体稀释剂组合,以形成组合的原料;引导所述组合的原料与在加氢处理条件下在加氢脱氧中具有催化活性的材料接触,以提供经加氢脱氧的中间产物;将所述经加氢脱氧的中间产物分离成至少两个馏分:蒸汽馏分和液体馏分;任选地提供一定量的所述液体馏分作为所述液体稀释剂;引导至少一定量的所述液体馏分与在异构化条件下在异构化中具有催化活性的材料接触,以提供经异构化的中间产物;将经异构化的中间产物分馏,以至少提供适合用作喷气燃料的烃和底部馏分;引导至少一定量的所述底部馏分与在加氢裂化条件下在加氢裂化中具有催化活性的材料接触,以提供经加氢裂化的中间产物,其相关的益处是,所述方法非常适合于将较高沸点的可再生原料有效地转化为较低沸点的产物,例如非化石煤油。除了所述喷气燃料之外,还可以生产柴油和其他烃。
在另一个实施方案中,根据ASTM D86,所述适合用作喷气燃料的烃馏分的最终沸点为小于300℃,其相关的益处是,所述方法的产物满足可再生喷气燃料规格ASTM D7566的沸点规范。
在另一个实施方案中,任选地通过添加包含一种或多种硫化合物(例如二甲基二硫化物或化石燃料)的流,相对于被引导与在加氢脱氧中具有催化活性的材料接触的组合的原料的气相中的分子氢的体积,硫化氢的总体积为至少50ppmv、100ppmv或200ppmv,其相关的益处是,所述方法用低成本的包含硫化的基础金属的在加氢脱氧中具有催化活性的材料有效地操作。
在另一个实施方案中,任选地通过添加包含一种或多种硫化合物(例如二甲基二硫化物或化石燃料)的流,相对于被引导与在加氢裂化中具有催化活性的材料接触的总流的气相中的分子氢的体积,硫化氢的总体积为至少50ppmv、100ppmv或200ppmv,其相关的益处是,能够使用廉价的包含硫化的基础金属的在加氢裂化中具有催化活性的材料。
在另一个实施方案中,所述原料包含至少50wt%的甘油三酸酯或脂肪酸,其相关的益处是,这样的原料非常适合于提供具有优异性质的喷气燃料。
在另一个实施方案中,加氢脱氧条件包括250-400℃的温度、30-150巴的压力和0.1-2的液时空速(LHSV),并且其中在加氢脱氧中具有催化活性的材料包含负载在载体上的一种或多种硫化的金属,所述金属选自镍、钴、钼或钨,所述载体包含一种或多种耐热氧化物,例如氧化铝、二氧化硅或二氧化钛,其相关的益处是,这样的工艺条件非常适合以成本有效的方式从可再生原料中去除杂原子,尤其是氧。
在另一个实施方案中,加氢裂化条件包括250-425℃的温度、30-150巴的压力以及0.5-4的液时空速(LHSV),任选地同时通过用冷的氢、进料或产物进行骤冷来进行中间冷却,并且其中在加氢裂化中具有催化活性的材料包含:(a)一种或多种活性金属,其选自铂、钯、镍、钴、钨和钼;(b)酸性载体,其选自显示高裂化活性且具有例如MFI、BEA和FAU的拓扑结构的分子筛以及无定形酸性氧化物,例如二氧化硅-氧化铝;和(c)耐热载体,例如氧化铝、二氧化硅或二氧化钛,或其组合,其相关的益处是,这样的工艺条件非常适合于降低产物的沸点以匹配煤油的沸点范围。
在另一个实施方案中,与所述底部馏分相比,所述经加氢裂化的中间产物中沸点为300℃以上的物质的量减少了至少20%wt、50%wt或80%wt或更多,其相关的益处是,由于高的工艺严苛性,高转化率使沸点为300℃以上的产物最小化。
在另一个实施方案中,引导至少一定量的所述经异构化的中间产物与在加氢脱芳构化条件下在加氢脱芳构化中具有催化活性的材料接触,以提供包含少于1wt/wt%、0.5wt/wt%或0.1wt/wt%的经加氢脱芳构化的产物,该百分数通过芳族分子的总质量相对于流中的所有烃来计算,其相关的益处是,这样的方法的产物满足喷气燃料规范ASTMD7566。所述在加氢脱芳构化条件下在加氢脱芳构化中具有催化活性的材料可以是在有利于加氢脱芳构化的中等温度下操作的在异构化中具有催化活性的材料。加氢脱芳构化条件优选地包括至少50%或80%的芳族化合物转化率。
在另一个实施方案中,加氢脱芳构化条件包括200-350℃的温度、30-150巴的压力以及0.5-8的液时空速(LHSV),其中所述在加氢脱芳构化中具有催化活性的材料包含:活性金属,其选自铂、钯、镍、钴、钨和钼,优选为一种或多种元素贵金属,例如铂或钯;以及耐热载体,优选为无定形二氧化硅-氧化铝、氧化铝、二氧化硅或二氧化钛,或其组合,其相关的益处是,这样的工艺条件适于芳族化合物的加氢。
在另一个实施方案中,引导包含至少90%vol氢的富氢流与在加氢脱芳构化中具有催化活性的材料接触,其相关的益处是,将总的工艺所要求的高纯度氢引导至加氢脱芳构化步骤,以有助于平衡向远离芳族化合物的方向移动。
在另一个实施方案中,异构化条件包括250-400℃的温度、30-150巴的压力以及0.5-8的液时空速(LHSV),并且其中在异构化中具有催化活性的材料包含:活性金属,其选自铂、钯、镍、钴、钨和钼,优选为一种或多种元素贵金属,例如铂或钯;酸性载体,优选为分子筛,更优选为具有选自MOR、FER、MRE、MWW、AEL、TON和MTT的拓扑结构;以及无定形耐热载体,其包含一种或多种选自氧化铝、二氧化硅、二氧化钛或其组合的氧化物,其相关的益处是,这样的条件和材料对于调节产物的冷流性质而言是成本有效和选择性的方法。
本公开的另一方面涉及一种用于由含氧化合物原料生产适合用作喷气燃料的烃馏分的工艺设备,所述工艺设备包括加氢裂化工段、加氢脱氧工段、分离工段、异构化工段和分馏工段,所述工艺设备被配置用于将原料、经加氢裂化的中间产物以及任选的液体稀释剂引导至加氢脱氧工段,以提供经加氢脱氧的中间产物;被配置用于在所述分离工段中将所述经加氢脱氧的中间产物分离为蒸汽馏分和液体馏分;被配置用于引导至少一定量的所述液体的经加氢脱氧的中间产物与在异构化条件下在异构化中具有催化活性的材料接触,以提供中间的经异构化的产物;并且被配置用于在所述分馏工段中分馏所述经异构化的中间产物,以至少提供适合用作喷气燃料的烃馏分和重质产物;引导至少一定量的所述底部产物与在加氢裂化下在加氢裂化中具有催化活性的材料接触,以提供所述经加氢裂化的中间产物,其相关的益处是,这样的工艺设备适合于进行所公开的方法,以成本有效和选择性地生产喷气燃料。
本公开中描述的方法接收可再生原料和/或含氧化合物原料,其包含一种或多种选自甘油三酸酯、脂肪酸、树脂酸、酮、醛、醇、酚和芳族羧酸的含氧化合物,其中所述含氧化合物源自一种或多种生物来源、气化过程、热解过程、Fischer-Tropsch合成、基于甲醇的合成或其他合成工艺,特别是得自可再生来源的原材料,例如源自植物、藻类、动物、鱼类、植物油的提炼、生活垃圾、废弃食用油(used cooking oil)、塑料废物、橡胶废物或工业有机废物,如妥尔油或黑液。这些原料中的一些可能含有芳族化合物;特别是通过热解或其他工艺从例如木质素和木材得到的产物或来自例如煎炸油的废品。取决于来源,含氧化合物原料可以包含1wt/wt%至40wt/wt%。生物来源通常将包含约10wt/wt%,并且衍生产物包含1wt/wt%至20wt/wt%或甚至40wt/wt%。
为了将可再生原料和/或含氧化合物原料转化为烃类运输燃料,引导原料与氢一起与在加氢处理(尤其是加氢脱氧)中具有催化活性的材料接触。尤其是在升高的温度下,催化加氢脱氧过程可能会发生副反应,例如从原料中的烯烃分子形成重质产物。为了缓和热量的释放,可以添加液态烃,例如液态再循环流或外部稀释进料。如果该方法被设计用于化石原料和可再生原料的共处理,则方便的是使用化石原料作为稀释剂,因为在化石原料的加工过程中释放的热量更少,因为释放更少的杂原子并且使更少的烯烃饱和,但是,根据本公开,通过使一种或多种液态烃再循环来缓和热量的释放。除了使温度缓和之外,再循环或稀释剂还具有降低烯烃物质聚合的可能性的作用。所得产物流将是经加氢脱氧的中间产物流,其包含烃(通常为正构石蜡)和酸性气体(例如CO、CO2、H2O、H2S、NH3)以及轻质烃(尤其是C3和甲烷)。
通常,加氢脱氧包括引导原料与催化活性材料接触,该催化活性材料通常包含负载在载体上的一种或多种硫化的金属,所述金属选自镍、钴、钼或钨,所述载体包含一种或多种耐热氧化物,通常为氧化铝,但可能是二氧化硅或二氧化钛。载体通常是无定形的。催化活性材料可以包含其他组分,例如硼或磷。条件通常是250-400℃的温度、30-150巴的压力以及0.1-2的液时空速(LHSV)。加氢脱氧通常是放热的,并且在存在大量氧的情况下,该方法可以涉及中间冷却,例如用冷的氢气、原料或产物进行骤冷。原料可以优选地包含一定量的硫以确保金属的硫化,以便保持其活性。如果气相包含少于10、50或100ppmv的硫,则可以向进料中添加硫化物供体,例如二甲基二硫化物(DMDS)。
对于待用作煤油馏分的经加氢脱氧的中间产物流,必须调节沸点范围。如果产生大量的重质中间产物,也可能需要调节沸点。通过引导经加氢脱氧的中间产物与在加氢裂化中具有催化活性的材料接触从而将长链石蜡加氢裂化为短链石蜡来调节沸点。为了确保最高的总选择性,仅将最终产物的重质馏分再循环,以用于加氢裂化。
加氢裂化包括引导经加氢脱氧的中间原料与在加氢裂化中具有催化活性的材料接触。在加氢裂化中具有催化活性的材料通常包含:活性金属(在本公开中,其为一种或多种硫化的基础金属,所述基础金属例如镍、钴、钨和/或钼);酸性载体(通常是显示高裂化活性并具有诸如MFI、BEA和FAU的拓扑结构的分子筛,但也可以使用无定形酸性氧化物,例如二氧化硅-氧化铝);和耐热载体(例如氧化铝、二氧化硅或二氧化钛,或其组合)。催化活性材料可以包含其他组分,例如硼或磷。优选的加氢裂化催化剂包含分子筛,例如ZSM-5、Y沸石或β沸石。
根据本公开,在加氢裂化中具有催化活性的材料可以包括基础金属或贵金属,并且位于在加氢脱氧中具有催化活性的材料的上游,其益处是,提供了经加氢裂化的中间产物作为加氢处理的稀释剂,只有材料。任选地,如果需要比加氢裂化产物更高量的稀释剂来控制加氢脱氧中的热量释放,则还可以将一定量的加氢脱氧产物再循环。
条件通常是250-400℃的温度、30-150巴的压力以及0.5-4的液时空速(LHSV)。由于加氢裂化是放热的,因此该方法可能涉及中间冷却,例如通过用冷的氢气、原料或产物进行骤冷。在加氢裂化中具有催化活性的材料上的一种或多种活性金属是基础金属,因此通常引导包含气相的中间经加氢脱氧的原料与在加氢裂化中具有催化活性的材料接触,而不进行进一步纯化。该混合物的该气相应当优选地含有至少50ppmv的硫。
为了在实践中将经加氢脱氧的中间产物用作燃料,必须调节凝固点。通过引导经加氢脱氧的中间产物与在异构化中具有催化活性的材料接触从而将正构石蜡异构化为异构石蜡来调节凝固点。
在异构化中具有催化活性的材料通常包含:活性金属(根据本公开,其为一种或多种元素贵金属,例如铂和/或钯);酸性载体(通常是显示高形状选择性并且具有诸如MOR、FER、MRE、MWW、AEL、TON和MTT的拓扑结构的分子筛);和通常为无定形的耐热载体(例如氧化铝、二氧化硅或二氧化钛,或其组合)。催化活性材料可以包含其他组分,例如硼或磷。优选的异构化催化剂包含分子筛,例如EU-2、ZSM-48、β沸石以及β沸石和沸石Y的组合。
通常,异构化包括引导经中间加氢脱氧的原料与在异构化中具有催化活性的材料接触。条件通常是250-350℃的温度、30-150巴的压力以及0.5-8的液时空速(LHSV)。异构化基本上是热中性的,因此在异构化反应器中通常不添加过量的氢气,但是需要存在一些氢气以进行异构化。由于在异构化中具有催化活性的最具选择性的材料上的活性金属是贵金属,因此经加氢脱氧的原料通常通过气/液分离进行纯化,以将硫、氮和碳氧化物的含量降至低于1-10ppm摩尔。
不饱和脂肪酸的加氢脱氧可能会产生芳族化合物作为副反应。因此,即使对于包含少于1%的芳族化合物的含氧化合物原料,也可能进一步需要引导经异构化的产物与在加氢脱芳构化中具有催化活性的材料接触。
在某些情况下,加氢脱芳构化可以于在加氢异构化中具有催化活性的材料的存在下令人满意地进行,但是也可能需要有一个单独的反应器或反应器床,该反应器或反应器床具有在加氢脱芳构化中具有催化活性的材料。
这种在加氢脱芳构化中具有催化活性的材料通常包含:活性金属(通常是元素贵金属,例如铂和/或钯,但也可以是硫化的基础金属,所述基础金属例如镍、钴、钨和/或钼);和耐热载体(例如无定形的二氧化硅-氧化铝、氧化铝、二氧硅或二氧化钛,或其组合)。加氢脱芳构化是平衡控制的,其中高温有利于芳族化合物,因此优选贵金属作为活性金属,因为与基础金属相比,贵金属在较低的温度下具有活性。
通常,加氢脱芳构化涉及引导中间产物与在加氢脱芳构化中具有催化活性的材料接触。由于在升高的温度下,芳族化合物和饱和分子之间的平衡向芳族化合物方向移动,因此优选中等温度。条件通常是200-350℃的温度、30-150巴的压力以及0.5-8的液时空速(LHSV)。在加氢脱芳构化中具有催化活性的材料上优选的活性金属通常优选为贵金属,因为与基础金属催化剂相比,通常贵金属催化剂在更低的温度下具有活性。也可以使用基础金属催化剂,并且在这种情况下,与中间经加氢脱氧的原料相关的气相优选地含有至少50ppmv的硫。通常在350℃以下的温度下操作的加氢裂化或加氢异构化催化剂将能够催化中等程度的加氢脱芳构化,例如将10%wt的芳族化合物减少到0.5%wt以下的芳族化合物。
这种必须组合3或4种催化活性材料以将可再生原料转化为喷气燃料自然使工艺布局复杂化,并且必须仔细考虑材料的顺序。另外,再循环可以用于三个不同的目的:气体再循环以有效利用氢气、液体围绕着在加氢裂化中具有催化活性的材料再循环以使煤油馏分的产率最大化、液体围绕着在加氢脱氧中具有催化活性的材料再循环以限制由于放热的加氢脱氧反应引起的温度升高。
当使用包含贵金属的催化活性材料进行异构化和加氢脱芳构化时,在此反应之前去除“酸性气体”,包括硫化氢和氨。也可以将一定量的经加氢脱氧的中间产物再循环至加氢脱氧反应器的入口。
根据当前的公开内容进行操作,其中围绕着加氢脱氧和加氢裂化反应器进行再循环,具有的优点是,允许通过多次通过而不是在苛刻条件下获得高的加氢裂化转化率,从而允许在中等温度下进行完全转化,因此保持高的煤油产率,并将过度裂化成石脑油和更轻质部分最小化。使用异构化催化剂来改善喷气燃料的凝固点,可以增加喷气燃料的蒸馏终点,同时仍满足凝固点要求。最后,由于第二阶段将使芳族化合物饱和,因此不要求第一阶段满足任何芳族化合物要求,从而允许第一阶段处理重质和/或更多的芳族化合物、环烷烃(naphthenic)或不饱和原料以及诸如废弃食用油、热解产物或妥尔油沥青的原料(其含有芳族化合物或不饱和原料,其在通常的加氢处理条件下可能产生少量芳族化合物),因为这些芳族化合物将在第二阶段被饱和。
根据本公开的一个实施方案对应于以下方法,其中将包含含氧化合物的流和包含一定量的硫的中间的经加氢裂化的流引导至加氢脱氧反应器,该加氢脱氧反应器含有催化活性材料,该催化活性材料包含一种或多种基础金属和具有低酸度的耐热载体。这样的材料在加氢脱氧和除去杂原子和双键的其他加氢处理反应中具有活性。中间的经加氢裂化的流起到散热剂(heat sink)的作用,吸收从加氢脱氧释放的反应热,从而在加氢脱氧反应器中保持中等的温度。该步骤提供了包含大量饱和直链烷烃,还有中间经加氢裂化的流,以及一定量的水、CO、CO2、甲烷、硫化氢和氨。
将经加氢脱氧的烃流引导至分离工段,抽出水、硫化氢和氨,并提供一种无酸的(sweet)烃流。将一定量的无酸的烃流任选地作为无酸的再循环烃进行再循环,并将一定量作为进料引导至异构化反应器中,该异构化反应器含有在异构化中具有催化活性的材料和任选的在加氢脱芳构化中具有催化活性的材料。这两种材料均基于贵金属催化剂(例如铂、钯或其组合)与酸性载体的组合。对于异构化,酸性载体优选为形状选择性的,以提供选择性的异构化,将直链烷烃重排为支链烷烃,同时使更轻质烃的产生最小化。对于加氢脱芳构化,酸性载体也有助于反应,此外,由于贵金属的活性高于基础金属,因此反应将在较低的温度下进行。由于芳族化合物和非芳族化合物之间的平衡在低温下会朝远离芳族化合物的方向移动,因此贵金属提供了与平衡相匹配的较低温度的优势。加氢脱芳构化甚至可能在在异构化中具有催化活性的材料(其经常会具有一定的加氢脱芳构化活性)上发生。
由于无酸的烃流不含有硫化氢或氨,因此在异构化中具有催化活性的材料的贵金属功能和酸功能均不受干扰,并且以高选择性生产了支链烃流。
将经异构化的流引导至分馏器(在分离器列中适当除去气相之后),并至少抽出气体馏分、中间馏分和底部馏分。将流(优选一定量的底部产物)再循环至加氢裂化反应器。
该布局提供了原料向柴油、喷气燃料范围或更轻质产物的转化,因为一些或甚至所有重质的经加氢脱氧的烃都可以被加氢裂化,从而产生更轻质的产物。喷气燃料/柴油联合生产或仅柴油生产是可能的,并且沸点的转化主要在仅采用基础金属催化剂的加氢脱氧工段和采用基础金属催化剂或贵金属催化剂的上游加氢裂化工段中进行,从而能够在单个工艺位置添加DMDS形式的硫;当这两个工段均采用基础金属催化剂时,在加氢裂化工段上游,或者当该工段采用贵金属催化剂时,在加氢裂化工段下游。此外,与加氢裂化条件无关,通过在贵金属催化剂上进行异构化来选择性地调节凝固点。
根据本公开的实施方案(其中加氢裂化和加氢处理催化剂均为基础金属类型)的一个益处是简化了这种单元的启动,因为分离工段上游的组合的加氢处理/加氢裂化工段可以通过硫化而活化,而分离工段下游的异构化工段可以通过还原而活化。
如果希望只生产柴油而不生产喷气燃料,则不需要加氢裂化。在这种情况下,可以优选绕过加氢裂化反应器,或者,在该反应器之前冷却产物,以使其不再具有活性。可以将工艺设备配置为允许在短时间内进行这样的配置,例如通过设置适当的设备和在控制室中进行控制。
附图
图1示出了根据本公开的方法的简化图。
图2示出了根据现有技术的方法的简化图。
图3示出了根据现有技术的方法的简化图。
图1是示出根据本公开的布局的简化图,为了简化,省略了气态流的供应和分离的细节。将再循环的流(126)与一定量的富氢流(未示出)一起引导至在加氢裂化条件下运行的加氢裂化反应器(HDC),以提供经加氢裂化的中间产物(112),将其与可再生原料(102)组合,并作为加氢脱氧进料流(104),任选地与一定量的富氢流(未示出)一起,引导至加氢脱氧反应器(HDO),在此与在加氢处理条件下在加氢反应中具有催化活性的材料接触。这提供了经加氢脱氧的中间产物(106)。将经加氢脱氧的中间产物(106)引导至分离器工段(SEP)(为简单起见,该分离器工段被示为单个单元),将经加氢脱氧的中间产物分离为用于再循环的气流和液体的中间产物流(108)。任选地将液体的中间产物流(108)分流成再循环的稀释剂流去往加氢裂化或加氢脱氧反应器(未示出),并且将异构化反应器进料流(未示出)与基本上无硫的氢流(未示出)一起作为进料引导至异构化反应器(ISOM),在此与在异构化条件下在异构化中具有催化活性的材料和任选的在加氢脱芳构化条件下在加氢脱芳构化中具有催化活性的另一种材料接触,提供经异构化的产物(116),将该经异构化的产物引导至分馏工段(FRAC)(为了简化起见,该分馏工段作为单个单元显示),将经异构化的产物分离为轻质顶部流(120)、石脑油产物(122)、喷气燃料产物(124)和底部柴油馏分(126)。如所提及的,将一定量的底部柴油馏分(126)引导作为再循环的流。
经异构化的产物(116)可以任选地与在加氢脱芳构化条件下在加氢脱芳构化中具有催化活性的另一种材料(未示出)接触,以提供经异构化的产物。
图2以类似于图1的详细程度示出了现有技术的示例,为简化起见,省略了气态流的供应和分离的细节。将可再生原料(202)与再循环的稀释剂流(228)组合,并作为加氢脱氧进料流(204)与一定量的富氢流(未显示)一起引导至加氢脱氧反应器(HDO),在此与在加氢处理条件下在氢化反应中具有催化活性的材料接触。这提供了经加氢脱氧的中间产物(214),其被引导至加氢异构化反应器(ISOM),在此与在异构化条件下在异构化中具有催化活性的材料接触,提供脱蜡的中间产物(216)。将脱蜡的中间产物(216)引导至分馏工段(FRAC)(为简化起见,将其作为单个单元显示),将经加氢裂化的产物分离为轻质顶部流(220)、石脑油流(222)、喷气燃料产物(224)和底部柴油馏分,该底部柴油馏分被分流成再循环的稀释剂流(228)和柴油产物流(226)。
图3示出了现有技术的另一示例,为简化起见,省略了气态流的供应和分离的细节。将可再生原料(302)与再循环的稀释剂流(328)组合,并作为经加氢脱氧的进料流(304)与一定量的富氢流(未示出)一起引导至加氢脱氧反应器(HDO),其在此与在加氢处理条件下在加氢化反应中具有催化活性的材料接触。这提供了经加氢脱氧的中间产物(306),其被引导至分离器(SEP),从中回收经纯化的经加氢脱氧的中间产物(308),将该中间产物(308)分流成再循环的稀释剂流(328)和异构化进料流(310),将异构化进料流(310)与无硫的氢流(未示出)组合并引导至加氢异构化反应器(ISOM)。在该反应器中,使组合的进料流与基于贵金属的在异构化条件下在异构化中具有催化活性的材料接触,提供脱蜡的中间产物(312)。将脱蜡的中间产物(312)引导至分馏工段(FRAC)(为简化起见,将其显示为单个单元),将经加氢裂化的产物分离为轻质顶部流(320)、石脑油流(322)、喷气燃料产物(324)和底部柴油馏分(326)。
实施例
比较了图1和图3所示的工艺布局的性能。
表1示出了可再生原料的特征,该可再生原料是动物脂肪和食用油以及加氢处理后的中间产物的组合。中间产物以C16和C18烷烃为主,具有高凝固点(24℃),并包含大于1.5wt/wt%的芳族化合物。将原料分别按照图1和图3的两个方法进行处理,该处理的结果示于表2,其中“实施例1”对应于图1,“实施例2”对应于图2。“净喷气燃料量”的值通过下式被计算为方法中产生的喷气燃料的量减去原料中已经存在的喷气燃料的量:净喷气燃料量=[总喷气燃料产物]-[进料中存在的原有喷气燃料]。
产率在该表中表示为进入该单元的进料的wt/wt%。例如,51wt/wt%的喷气燃料产率表明在该单元中每处理100kg进料,就会产生51kg的喷气燃料。
两个实施例的结果均显示具有优异性质、低凝固点(-40℃)和低芳族化合物含量(<0.5%wt)的喷气燃料的生产。假定喷气燃料和柴油之间的分馏界限为300℃,根据本公开的实施例1具有54wt/wt%的喷气燃料产率,而实施例2具有43wt/wt%的喷气燃料产率。在喷气燃料价值更高的假设下进行的工艺优化中,这种差异显然是实施例1极具吸引力的优势。改善的产率是由于高沸点柴油在加氢裂化反应器中向喷气燃料的转化。
表1
Claims (13)
1.一种用于由含氧化合物原料(102)生产适合用作喷气燃料(124)的烃馏分的方法,该方法包括以下步骤:
a.将原料(102)与一定量的经加氢裂化的中间产物(112)和任选的液体稀释剂组合以形成组合的原料(104),引导所述组合的原料(104)与在加氢处理条件下在加氢脱氧(HDO)中具有催化活性的材料接触,以提供经加氢脱氧的中间产物(106);
b.将所述经加氢脱氧的中间产物(106)分离为包括蒸汽馏分和液体馏分(108)的至少两个馏分;
c.任选地提供一定量的所述液体馏分(108)作为所述液体稀释剂,引导至少一定量的所述液体馏分(108)与在异构化条件下在异构化(ISOM)中具有催化活性的材料接触,以提供经异构化的中间产物(116);
d.将所述经异构化的中间产物(116)分馏,以至少提供适合用作喷气燃料的烃馏分(124)和底部馏分(126);
e.引导至少一定量的所述底部馏分(126)与在加氢裂化条件下在加氢裂化(HDC)中具有催化活性的材料接触,以提供经加氢裂化的中间产物(112)。
2.根据权利要求1或2所述的方法,其中根据ASTM D86,所述适合用作喷气燃料的烃馏分(124)的最终沸点为小于300℃。
3.根据权利要求1或2所述的方法,其中任选地通过添加包含一种或多种硫化合物例如二甲基二硫化物或化石燃料的流,相对于被引导与在加氢脱氧中具有催化活性的材料接触的组合的原料(104)的气相中的分子氢的体积,硫化氢的体积为至少50ppmv、100ppmv或200ppmv。
4.根据权利要求1、2或3所述的方法,其中任选地通过添加包含一种或多种硫化合物例如二甲基二硫化物或化石燃料的流(114),相对于被引导与在加氢裂化(HDC)中具有催化活性的材料接触的总流(116)的气相中的分子氢的体积,硫化氢的体积为至少50ppmv、100ppmv或200ppmv。
5.根据权利要求1、2、3或4所述的方法,其中所述原料(102)包含至少50%wt的甘油三酸酯或脂肪酸。
6.根据权利要求1、2、3或4所述的方法,其中加氢脱氧条件包括250-400℃的温度、30-150巴的压力和0.1-2的液时空速(LHSV),并且其中在加氢脱氧中具有催化活性的材料包含负载在载体上的一种或多种硫化的金属,所述金属选自镍、钴、钼或钨,所述载体包含一种或多种耐热氧化物,例如氧化铝、二氧化硅或二氧化钛。
7.根据权利要求1、2、3、4、5或6所述的方法,其中加氢裂化条件包括250-425℃的温度、30-150巴的压力和0.5-4的液时空速(LHSV),任选同时通过用冷的氢、进料或产物进行骤冷来进行中间冷却,并且其中在加氢裂化中具有催化活性的材料包含(a)一种或多种活性金属,其选自铂、钯、镍、钴、钨和钼;(b)酸性载体,其选自显示高裂化活性并具有例如MFI、BEA和FAU的拓扑结构的分子筛以及无定形酸性氧化物,例如二氧化硅-氧化铝;和(c)耐热载体,例如氧化铝、二氧化硅或二氧化钛,或其组合。
8.根据权利要求1、2、3、4、5、6或7所述的方法,其中与所述底部馏分(126)相比,所述经加氢裂化的中间产物(112)中沸点为300℃以上的物质的量减少了至少20%wt、50%wt或80%wt或更多。
9.根据权利要求1、2、3、4、5、6、7或8所述的方法,其中引导至少一定量的所述经异构化的中间产物(116)与在加氢脱芳构化条件下在加氢脱芳构化(HDA)中具有催化活性的材料接触,以提供包含少于1wt/wt%、0.5wt/wt%或0.1wt/wt%的经加氢脱芳构化的产物,该百分数通过芳族分子的总质量相对于流中的所有烃来计算。
10.根据权利要求9所述的方法,其中加氢脱芳构化条件包括200-350℃的温度、30-150巴的压力以及0.5-8的液时空速(LHSV),其中所述在加氢脱芳构化中具有催化活性的材料包含:活性金属,其选自铂、钯、镍、钴、钨和钼,优选一种或多种元素贵金属,例如铂或钯;以及耐热载体,优选无定形二氧化硅-氧化铝、氧化铝、二氧化硅或二氧化钛,或其组合。
11.根据权利要求8、9或10所述的方法,其中引导包含至少90%vol氢的富氢流与在加氢脱芳构化(HDA)中具有催化活性的材料接触。
12.根据权利要求1、2、3、4、5、6、7、8、9、10或11所述的方法,其中异构化条件包括250-350℃的温度、30-150巴的压力以及0.5-8的液时空速(LHSV),并且其中在异构化中具有催化活性的材料包含:活性金属,其选自铂、钯、镍、钴、钨和钼,优选为一种或多种元素贵金属,例如铂或钯;酸性载体,优选为分子筛,更优选为具有选自MOR、FER、MRE、MWW、AEL、TON和MTT的拓扑结构;以及无定形耐热载体,其包含一种或多种选自氧化铝、二氧化硅、二氧化钛或其组合的氧化物。
13.一种用于由含氧化合物原料(102)生产适合用作喷气燃料的烃馏分(124)的工艺设备,所述工艺设备包括加氢裂化工段(HDC)、加氢脱氧工段(HDO)、分离器工段、异构化工段(ISOM)和分馏工段(FRAC),所述工艺设备被配置用于
a.将再循环的产物(126)引导至加氢裂化工段(HDC),以提供经加氢裂化的中间产物(112);
b.将原料(102)、所述经加氢裂化的中间产物(112)以及任选的另外的再循环的液体稀释剂(126)引导至加氢脱氧工段(HDO),以提供经加氢脱氧的中间产物(106);
c.在所述分离器工段(SEP)中将所述经加氢脱氧的中间产物(106)分离为蒸汽馏分和液体馏分(108);
d.引导至少一定量的所述液体的经加氢脱氧的中间产物(108)与在异构化条件下在异构化(ISOM)中具有催化活性的材料接触,以提供中间的经异构化的产物(116);和
e.在所述分馏工段(FRAC)中分馏所述经异构化的中间产物(116),以至少提供适合用作喷气燃料的烃馏分(124)和所述再循环的产物(126)。
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