CN114341320B - 烃组合物 - Google Patents

烃组合物 Download PDF

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CN114341320B
CN114341320B CN202080061391.1A CN202080061391A CN114341320B CN 114341320 B CN114341320 B CN 114341320B CN 202080061391 A CN202080061391 A CN 202080061391A CN 114341320 B CN114341320 B CN 114341320B
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hydrocarbon composition
fuel
paraffins
hydrocarbon
isomerized
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CN114341320A (zh
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卡蒂·赞德贝格
瓦艾诺·西波拉
珍妮·苏普拉
杰西·维尔亚
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Neste Oyj
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  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Liquid Carbonaceous Fuels (AREA)

Abstract

公开了一种包括异构化链烷烃的烃组合物，所述烃组合物在蒸馏曲线中具有特定的截止点，密度为768.0至772.0，且平均碳数为14.3至15.1。烃组合物可用作燃料或燃料组分，尤其是喷气燃料。还公开了一种生产烃组合物的方法。烃组合物中的异构化链烷烃可以来自可再生源。

Description

烃组合物
技术领域
本发明总体上涉及一种包含异构化链烷烃的烃组合物，特别地涉及一种具有优异凝固点(freezing point，冰点)且可用作航空燃料中的组分或用作航空燃料的烃组合物。
背景技术
喷气燃料或航空燃料是一种旨在用于燃气涡轮发动机驱动的航空器的燃料。最常用的航空燃料Jet A和Jet A-1是按照标准化的国际规范生产的。喷气燃料是不同烃的混合物。其尺寸、分子量或碳数取决于产品规范要求的物理性质，例如闪点、凝固点、沸程。煤油型喷气燃料(包括Jet A和Jet A-1)通常具有每个分子约8至16个碳原子的碳数分布。
化石燃料或石油基燃料可以至少部分地被生物源或其他可再生源燃料所取代。由于减少GHG、CO2等的排放的全球倡议，可再生航空燃料需求在未来不断增长。一个可能的关键解决方案是增加可再生燃料在航空燃料中的使用。来自生物源的燃料可包括可再生原料，例如脂肪和/或油。可以从这些含三酰甘油的原料中获得几种类型的燃料。可以从脂质原料中获得的产品的一个实例是，在催化剂的存在下，通过在升高的温度和压力下的加氢脱氧反应从脂肪或油中产生的燃料。
在组成满足燃料规范之前，从含三酰甘油的原料的加氢脱氧反应形成的烃通常需要进行异构化。烃的异构化降低了烃的熔点，从而改善组合物的冷流性能。烃的异构化是加氢裂化的形式，并且在广泛的异构化条件下，存在降低烃碳数的风险。
从可再生源中生产烃航空燃料的其他方法包括加氢裂化(有或没有异构化)。可能需要对由可再生源生产的烃进行分馏以生产具有良好凝固点的航空燃料。
公开WO 2018/224730描述了一种多用途燃料组合物，其包含石油基(petroleumbased，基于石油的，石油类)喷气燃料组分和可再生喷气燃料组分，其中燃料组合物具有-40℃的凝固点。可再生喷气燃料组分包含异构化链烷烃和正链烷烃，其来源于植物油或动物脂肪。
公开WO 2005/026297描述了一种燃料组合物，其包含石油基煤油燃料和费托衍生煤油燃料，包含正链烷烃和异链烷烃。公开中描述的费托衍生煤油组分具有通常为730至770kg/m3的密度。
航空燃料的低温性能对于确保航空器充分可靠的***运行至关重要。航空燃料的凝固点是确保在所有条件下燃料的可泵性的重要性能。
满足航空燃料性能的组分产率也很重要，尤其是当组分由生物或可再生源生产时。燃料组分的密度是用于流量计算、燃料装载、燃料箱设计、计量装置等的重要性能。燃料密度变化对确定航空器装载重量和可达到的范围有重大影响。
发明内容
因此，本发明的一个目的是提供一种烃组合物，该烃组合物具有增加的产率和密度、优异的凝固点以及使该组合物能够用作航空燃料或航空燃料中的组分的组合物性能。
根据本发明的一个方面，提供了一种包含异构化链烷烃的烃组合物，其中
-烃组合物具有的T10(℃)截止温度(cut-off temperature)为185至205℃，T90(℃)截止温度为270至295℃，且最终沸点(℃)为275至300℃，以及
-烃组合物的密度为768.0至772.0kg/m3，且
-烃组合物中的烃的平均碳数为14.3至15.1。
根据本发明的另一方面，提供了一种包含根据本发明的烃组合物的燃料或燃料组分。
根据本发明的另一方面，提供了一种制备根据本发明的烃组合物的方法。
本发明的实施方式在从属权利要求和下面的详细描述中定义。
根据本发明的烃组合物的优点在于，该组合物具有高密度结合优异的凝固点。这种组合能实现灵活共混该组分与石油基航空燃料。航空燃料组分的优异凝固点在长途飞行中也很有利，尤其是在高海拔地区。具有优异凝固点的航空燃料也可在极端天气条件下使用，并在所有条件下提供安全使用，这可能是一个益处，例如用于军事用途。
具体实施方式
喷气燃料或航空燃料是旨在用于燃气涡轮发动机驱动的航空器的燃料。喷气燃料需要满足某些物理性能以被分类为喷气燃料。喷气燃料的定义标准包括至少DEF STAN 91-091(2018)、ASTM D1655-19(Jet A-1)和ASTM D7566-19。
喷气燃料最重要的性能之一是凝固点。凝固点是对温热组合物时可见固体燃料蜡颗粒消失的温度的测量，该组合物已冷却到可见颗粒出现的温度。Jet A(ASTM D1655-19)标准喷气燃料的凝固点必须为至少-40℃，对于Jet A-1燃料为至少-47℃。密度是任何燃料的另一个重要性能，尤其是对于喷气燃料。
烃组合物的低凝固点通常与具有较低碳数的烃相关联。具有较低碳数的烃也具有较低密度。因此，与具有较长链长度的链烷烃相比，短链长度的链烷烃具有较低密度。然而，短链链烷烃的凝固点较低。
令人惊讶的是，现在已经获得了具有高密度和低凝固点的烃组合物，其满足喷气燃料规范。这是通过设置烃组合物的蒸馏曲线的某些截止点来实现的。
因此，本发明的一个实施方式是包含异构化链烷烃的烃组合物，该组合物具有蒸馏曲线的某些截止点和高密度。烃组合物的凝固点满足等于或低于-40℃的喷气燃料规范。
烃组合物在此是指主要包含烃的组合物，即仅包含碳和氢原子的有机分子。烃组合物可以含有少量的含有诸如硫的杂原子的分子。根据本发明的烃组合物可用作燃料组分，尤其是用作喷气燃料组分。
根据本发明的烃组合物包含异构化链烷烃(或i-链烷烃或iso-链烷烃)。异构化链烷烃在此是指具有一个或多个侧链的链烷烃。侧链通常为甲基、乙基和丙基取代基的形式，并且可以位于链烷烃链上的任何位置。异构化链烷烃可以通过正链烷烃(n-链烷烃)的异构化来生产。异构化链烷烃可以来自任何来源。异构化链烷烃来源的非限制性实例为脂肪酸加氢脱氧生产的烃或费托法生产的烃。
本发明涉及一种烃组合物，其T10(℃)截止温度为185℃至205℃。该组合物的T90(℃)截止温度为270℃至295℃，最终沸点(℃)为275℃至300℃。收集的馏分的蒸馏条件和性质随用于生产异构化链烷烃的方法和使用的可再生源而变化。本领域技术人员熟知各种蒸馏和分馏方法，并且可优化获得根据本发明的烃组合物所需的条件。
根据本发明的烃组合物具有768.0kg/m3至772.0kg/m3的密度。在本发明的另一个实施方式中，烃组合物的密度为770.0kg/m3至772.0kg/m3，并且在另一个实施方式中，密度为771.0kg/m3至772.0kg/m3。应将密度范围解释为包括等于范围端点的密度。应注意的是，即使烃组合物的密度略有增加，也会产生显著影响。组合物的密度越高，意味着每体积有更多的能量和更高的热值(卡值)。这在燃料应用中尤其重要，因为燃料罐的容量总是有限的。此外，当烃组合物与其他组分共混时，更高的密度也会带来益处。例如，喷气燃料的最小密度为775kg/m3(ASTM D7566)，如果可再生组分的密度更高，则石油基喷气燃料组分的密度具有更大的灵活性。
烃组合物的密度可以使用测量烃燃料组合物密度的任何标准化方法进行测量，如ASTM D4052。
在本发明的一个实施方式中，烃组合物包含平均碳数为14.3至15.1的烃。在另一个实施方式中，组合物中烃的平均碳数为14.5至15.1，并且在另一个实施方式中为14.7至15.0。碳数范围应解释为包括碳数等于范围端点的烃。
使用气相色谱法(GC)测量烃组合物中烃的平均碳数。GC法的条件在下表1中列出。
表1.用于测定烃的碳数的GC设置
令人惊讶的是，在不牺牲烃组合物的凝固点的情况下，可以获得具有高碳数和高密度的烃组合物。较高的碳数通常意味着较低的凝固点。
根据本发明的一个实施方式，碳数为14至17的烃组合物中的烃的量至少为全部烃含量的60wt-％。
根据本发明的一个实施方式，烃组合物包含异构化链烷烃，根据烃组合物的总链烷烃含量计算，异构化链烷烃超过90wt-％，优选超过92wt-％，且最优选超过95wt-％。异构化链烷烃主要是单异构化、双异构化或三异构化的，但一些链烷烃可具有更多的侧链。异构化链烷烃可为甲基、乙基或丙基取代的。根据本发明的烃组合物为各种异构化链烷烃的混合物。应注意的是，碳数不随异构化程度或侧链类型而变化。链烷烃中碳的数量保持不变。
高异构化程度能使本发明的烃组合物具有独特的性质。通常，较高的异构化程度意味着较低的凝固点。然而，异构化程度本身并不能充分解释本发明的烃组合物的低凝固点和高密度。
在本发明的一个方面中，烃组合物具有-40℃、或优选-43℃或更低的凝固点。通常，最低凝固点可为-60℃。最低可测量凝固点为-80℃。要求待用作喷气燃料的组合物的凝固点为-40℃或更低。航空燃料的凝固点根据标准IP529进行测量。显然，在所有可能的条件下，喷气燃料保持可泵送状态是非常重要的，以确保航空燃气涡轮发动机完全正常工作。特别地，当喷气燃料或喷气燃料组分由生物或可再生源生产时，有时可能难以达到所需的低凝固点。这在链烷烃可再生燃料组分中尤其困难，其中总产率很重要。
在本发明的一个方面中，烃组合物由可再生源(可再生原材料)生产。这里，术语可再生源或可再生原材料是指包括除从石油原油(化石基油或石油基油)中获得的那些以外的原料。本发明中可使用的可再生源包括但不限于来自植物和/或动物和/或鱼类和/或昆虫的生物油和脂肪，以及来自利用微生物(如藻类、细菌、酵母菌和霉菌)的方法的生物油和脂肪，合适的还包括衍生自所述脂肪和油及其混合物的化合物。产生生物油或脂肪的物种可以是天然的或基因改造的。生物油和脂肪可以是初压油和脂肪或回收油和脂肪。
含有脂肪酸和/或脂肪酸酯和/或脂肪酸衍生物的合适生物油为木基和其他植物基和蔬菜基脂肪和油，如菜籽油、菜油、芥花油、妥尔油、麻疯树籽油、葵花籽油、大豆油、***籽油、橄榄油、亚麻籽油、芥子油、棕榈油、花生油、蓖麻油、椰子油，以及通过基因操纵培育的植物中所含的脂肪、动物基脂肪如猪油、牛油、鲸油和牛奶中所含的脂肪，以及食品工业的回收脂肪和上述的混合物，以及源自利用微生物(如藻类、细菌、酵母菌和霉菌)的方法的脂肪和油。
可再生源还包括可回收的废油和脂肪或可回收的废油和脂肪的残留物。
适合用作新鲜进料的生物油和脂肪可包含C12-C24脂肪酸及其衍生物，例如酸酐或脂肪酸酯，以及脂肪酸的甘油三酯和甘油二酯或其组合。脂肪酸或脂肪酸衍生物如酯，可通过生物油的水解或甘油三酯的分馏或酯交换反应或利用微生物的微生物方法产生。
根据本发明的烃组合物的异构化链烷烃可以通过任何合适的方法生产。在一个实施方式中，链烷烃由可再生油(例如植物油或动物脂肪)产生，其经过脱氧过程以去除杂原子，主要是来自可再生油的氧。
在优选的实施方式中，对可再生原材料进行的脱氧处理为加氢处理。优选地，对可再生原料进行加氢脱氧(HDO)，其优选地使用HDO催化剂。催化HDO是最常见的除氧方法，并且已被广泛研究和优化。然而，本发明不限于此。作为HDO催化剂，可以使用包含负载在载体上的氢化金属的HDO催化剂。实例包括包含氢化金属的HDO催化剂，该氢化金属选由自Pd、Pt、Ni、Co、Mo、Ru、Rh、W或其组合组成的组。其中，氧化铝或二氧化硅适合用作载体。例如，可在100-500℃的温度和10-150巴(绝对)的压力下进行加氢脱氧步骤。
在一个实施方式中，异构化链烷烃组分通过从生物质气化开始的费托法生产。这种合成路线通常也被称为BTL，或生物质转化为液体。文献中充分证实，生物质，例如木质纤维材料，可以在高温下使用氧气或空气进行气化，以产生氢气和一氧化碳的气体混合物(合成气)。气体净化后，它可用作费托合成路线的原料。在费托合成中，链烷烃是由合成气生产的。费托链烷烃的范围从气态组分到蜡状链烷烃，且中间馏分沸程链烷烃可通过蒸馏从产品中获得。
通过加氢处理可再生油或费托法形成的正链烷烃需要进行进一步的异构化处理。异构化处理导致加氢处理的原料的烃链支化，即异构化。烃链的支化改善低温性能，即异构化处理形成的异构组合物比加氢处理的原料具有更好的低温性能。更好的低温性能是指凝固点的温度值较低。通过异构化处理形成的异构烃或异构化链烷烃可以具有一个或多个侧链或支链。
异构化步骤可以在异构化催化剂的存在下进行，并且任选地在添加到异构化过程的氢气的存在下进行。合适的异构化催化剂包含分子筛和/或选自周期表第VIII族的金属，以及任选的载体。优选地，异构化催化剂包含SAPO-11、或SAPO-41、或ZSM-22、或ZSM-23、或镁碱沸石(fernerite)，以及Pt、Pd或Ni、和Al203或Si02。典型的异构化催化剂为，例如，Pt/SAPO-11/Al203、Pt/ZSM-22/Al203、Pt/ZSM-23/Al203和Pt/SAPO-11/Si02。催化剂可以单独使用，或者组合使用。为了减少催化剂失活，添加的氢气的存在特别优选。
在优选的实施方式中，异构化催化剂是贵金属双功能催化剂，例如与氢气组合使用的Pt-SAPO和/或Pt-ZSM催化剂。例如，异构化步骤可在200-500℃、优选280-400℃的温度和5-150巴、优选10-130巴、更优选30-100巴(绝对)的压力下进行。异构化步骤可包括进一步的中间步骤，例如纯化步骤和分馏步骤。异构化可在例如300℃至350℃下进行。
在本发明的一个实施方式中，需要对异构化过程中形成的异构化链烷烃进行分馏，以获得根据本发明的烃组合物。如果形成的异构化链烷烃满足根据本发明的烃组合物的要求，则不需要对异构化链烷烃进行分馏。分馏可使用任何合适的方法进行，且不限于蒸馏。蒸馏是从烃组合物中分离各种馏分最常用的方法，也适用于这里。
根据另一方面，本发明还涉及包含根据本发明的烃组合物的燃料或燃料组分。在本发明的另一方面中，燃料或燃料组分是喷气燃料或喷气燃料组分。
在一个方面，本发明涉及一种喷气燃料，该喷气燃料含有根据本发明的烃组分，其含量至高达喷气燃料的50vol.％，且余量为石油基喷气燃料。优选地，喷气燃料含有根据本发明的烃组分，其浓度为3vol.％至50vol.％，更优选为5vol.％至45vol.％，甚至更优选为10vol.％至30vol.％。根据本发明的喷气燃料中的余量是石油基喷气燃料。术语“石油基喷气燃料”是指由满足至少一种喷气燃料规范的石油或原油生产的任何常规喷气燃料或航空燃料。喷气燃料或航空燃料的规范包括但不限于Jet A、Jet A-1(DEF STAN 91-91、ASTMD1655)和各种军用标准(JP-1至JP-8)。
根据另一方面，本发明还涉及生产根据本发明的烃组合物的方法。生产烃组合物的方法包括以下方法步骤：
-提供包含脂肪酸的可再生原料，
-对原料进行脱氧以生产链烷烃，
-将生产的链烷烃进行异构化步骤以生产异构化链烷烃，以及
-分馏生产的异构化链烷烃以获得根据本发明的烃组合物。
在一个实施方式中，分馏包括将根据本发明生产的异构链烷烃分馏为一个单一馏分，产率为至少20wt-％，优选产率为至少30wt-％，最优选产率为至少40wt-％。
实施例
实施例1(比较)
一种可再生的链烷烃产品是通过对蔬菜和动物脂肪来源的原料混合物进行重裂解加氢脱氧和异构化而生产的。使用各种分析方法对该产品进行分析(表2)。
表2.分析的可再生链烷烃产品。
分析 方法 单位 值
凝固点 IP529 ℃ -42.0
密度 ASTM D4052 kg/m3 753.0
加权平均碳数 NM490 - 12.0
％碳数14-17 NM490 wt-％ 30.5
T10(℃)截止温度 ASTM D86 ℃ 168.5
T90(℃)截止温度 ASTM D86 ℃ 245.5
最终沸点 ASTM D86 ℃ 256.0
表2中的分析产品满足喷气燃料规范的凝固点，但凝固点并不是异常低。
实施例2(比较)
一种可再生的链烷烃产品是通过对蔬菜和动物脂肪来源的原料混合物进行加氢脱氧和异构化而生产的。使用各种分析方法对该产品进行分析(表3)。
表3.分析的可再生链烷烃产品。
分析 方法 单位 值
凝固点 IP529 ℃ -41.0
密度 ASTM D4052 kg/m3 774.1
加权平均碳数 NM490 - 15.6
％碳数14-17 NM490 wt-％ 55.8
T10(℃)截止温度 ASTM D86 ℃ 210.0
T90(℃)截止温度 ASTM D86 ℃ 289.0
最终沸点 ASTM D86 ℃ 308.2
表3中的分析产品满足喷气燃料规范的凝固点，但凝固点并不是异常低。
实施例3
将通过对实施例2中的蔬菜和动物脂肪来源的原料混合物进行加氢脱氧和异构化而生产的可再生的链烷烃产品进一步引导至分馏单元。在分馏单元中，可再生链烷烃产品分为两个馏分。使用各种分析方法(表4)重新分析含有80wt-％的原始可再生链烷烃产品的馏分的轻馏分。
表4.分析的可再生链烷烃产品。
分析 方法 单位 值
凝固点 IP529 ℃ -49.1
密度 ASTM D4052 kg/m3 771.6
加权平均碳数 NM490 - 15.0
％碳数14-17 NM490 wt-％ 68.5
T10(℃)截止温度 ASTM D86 ℃ 198.6
T90(℃)截止温度 ASTM D86 ℃ 280.3
最终沸点 ASTM D86 ℃ 287.5
该分析产品满足高质量可再生航空燃料的所有要求。从分析结果可以看出，当链烷烃产品的密度低于772kg/m3(测量值为771.6kg/m3)时，与比较例2的产品相比，凝固点显著下降至-49.1℃。
实施例4
将通过对蔬菜和动物脂肪来源的另一原料混合物进行加氢脱氧和异构化而生产的另一可再生的链烷烃产品进一步引导至分馏单元。在分馏单元中，可再生链烷烃产品分为两个馏分。使用各种分析方法(表5)重新分析含有80wt-％的原始可再生链烷烃产品的馏分的轻馏分。
表5分析的可再生链烷烃产品。
该产品也满足高质量可再生航空燃料的所有要求。从分析结果可以看出，尽管事实上链烷烃组合物的密度超过768kg/m3(测量值为770.1kg/m3)，但凝固点(测量值为-50.9℃)显著低于比较例1的产品的凝固点。
对于本领域技术人员显而易见的是，随着技术的进步，本发明构思可以各种方式实现。本发明及其实施方式不限于上述实施例，而是可以在权利要求的范围内变化。

Claims (18)

1.一种包括异构化链烷烃的烃组合物，其中
-所述烃组合物具有185至205℃的T10截止温度、270至295℃的T90截止温度、以及275至300℃的最终沸点，并且
-使用标准ASTM D4052测量的所述烃组合物的密度为768.0至772.0kg/m3，并且
-所述烃组合物中的烃的平均碳数为14.3至15.1，并且
-根据所述烃组合物的总链烷烃含量计算，所述烃组合物包括超过90wt.％的异构化链烷烃。
2.根据权利要求1所述的烃组合物，其中，所述烃组合物的所述烃的平均碳数为14.5至15.1。
3.根据权利要求1或2所述的烃组合物，其中，所述烃组合物的密度为770.0至772.0kg/m3。
4.根据权利要求1或2所述的烃组合物，其中，至少60wt-％的所述烃组合物中的所述烃具有14至17的碳数。
5.根据权利要求1或2所述的烃组合物，其中，所述烃组合物具有低于-40℃的凝固点。
6.根据权利要求1所述的烃组合物，其中，所述烃组合物的所述烃的平均碳数为14.7至15.0。
7.根据权利要求1或2所述的烃组合物，其中，所述烃组合物的密度为771.0至772.0kg/m3。
8.根据权利要求1或2所述的烃组合物，其中，所述烃组合物具有低于-43℃的凝固点。
9.一种燃料或燃料组分，包含根据权利要求1至8中任一项所述的烃组合物。
10.根据权利要求9所述的燃料或燃料组分，其中，所述燃料或燃料组分为喷气燃料或喷气燃料组分。
11.根据权利要求9或10所述的燃料或燃料组分，其中，所述燃料为喷气燃料，所述喷气燃料包含高达50vol.％的根据权利要求1-8中任一项所述的烃组合物并且余量为石油基喷气燃料。
12.根据权利要求9或10所述的燃料或燃料组分，其中，所述燃料为喷气燃料，所述喷气燃料包含3vol.％至50vol.％的根据权利要求1-8中任一项所述的烃组合物并且余量为石油基喷气燃料。
13.根据权利要求9或10所述的燃料或燃料组分，其中，所述燃料为喷气燃料，所述喷气燃料包含5vol.％至45vol.％的根据权利要求1-8中任一项所述的烃组合物并且余量为石油基喷气燃料。
14.根据权利要求9或10所述的燃料或燃料组分，其中，所述燃料为喷气燃料，所述喷气燃料包含10vol.％至30vol.％的根据权利要求1-8中任一项所述的烃组合物并且余量为石油基喷气燃料。
15.一种生产权利要求1至8中任一项所述的烃组合物的方法，其中，所述方法包括以下步骤
-提供包括脂肪酸的可再生原料，
-对所述原料进行脱氧以生产链烷烃，
-将生产的所述链烷烃进行异构化步骤以生产异构化链烷烃，以及
-将生产的所述异构化链烷烃分馏以获得根据权利要求1至8中任一项所述的烃组合物。
16.根据权利要求15所述的方法，其中，所述分馏包括
-对生产的所述异构化链烷烃进行分馏，使得根据权利要求1至8中任一项所述的烃组合物作为单一馏分获得，所述单一馏分具有基于总异构化链烷烃含量计算的至少20wt-％的产率。
17.根据权利要求15所述的方法，其中，所述分馏包括
-对生产的所述异构化链烷烃进行分馏，使得根据权利要求1至8中任一项所述的烃组合物作为单一馏分获得，所述单一馏分具有基于总异构化链烷烃含量计算的至少30wt-％的产率。
18.根据权利要求15所述的方法，其中，所述分馏包括
-对生产的所述异构化链烷烃进行分馏，使得根据权利要求1至8中任一项所述的烃组合物作为单一馏分获得，所述单一馏分具有基于总异构化链烷烃含量计算的至少40wt-％的产率。
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