CN103189479B - 可再生生物馏分油的生产 - Google Patents
可再生生物馏分油的生产 Download PDFInfo
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Abstract
提供了一种方法和系统,用于从生物油中分离轻质馏分、生物馏分油馏分(组合物)和重质馏分,和用于生产包含至少部分生物馏分油组合物和稳定添加剂的可再生馏分油。该方法包括基于各自的沸点将生物油分离为轻质、生物馏分油和重质馏分。将至少一部分生物馏分油组合物和稳定剂与石油衍生柴油范围的物流不进行任何预先加氢处理共混,由此提供可再生馏分油组合物。
Description
技术领域
本发明总体上涉及从生物油中分离生物馏分油组合物的方法和系统。更具体地,本发明涉及包含至少部分生物馏分油组合物的可再生馏分油的生产。
背景技术
由于化石燃料不断升高的成本和环境忧虑,可再生能源变得日益重要。可再生燃料源的开发提供了减少对化石燃料依赖的途径。因此,许多不同领域的可再生燃料研究正在探索和发展。
由于成本低和可获得性广泛,生物质作为可再生燃料研究中理想的原料正受到越来越多的重视。所以,开发出许多使用生物质作为原料生产有用的生物燃料和/或专用化学品的不同的转化方法。现有的生物质转化方法包括例如燃烧、气化、慢速热解、快速热解、液化和酶转化。可从上述生物质转化方法获得的有用产品之一是通常称为“生物油”的液体产品。生物油可被处理成运输燃料、烃化学品和/或专用化学品。
尽管生物质转化方法近来取得了进展,但是许多现有的生物质转化方法生产的是氧含量高的低质生物油,这样的生物油难以(如果不是不可能的话)分离为多种馏分。由于生物油中的氧含量高,这些生物油需要大规模的二次提质以用作运输燃料和/或用作燃料添加剂。另外,这些得自生物油的运输燃料和/或燃料添加剂质量随生物油中原始氧含量而不同。
因此,需要改进的方法和系统,用来将生物油分离为多种馏分如生物馏分油,和将该馏分用作可再生燃料的共混组分。
发明内容
在一个实施方案中,本发明涉及一种生产生物馏分油组合物的方法,该方法包括:(a)在包含催化剂的转化反应器中转化生物质,由此生成包含蒸气转化产物的转化反应器流出物;(b)将至少一部分蒸气转化产物冷凝,由此提供总氧含量小于约15wt%的生物油;和(c)从生物油中分离生物馏分油组合物,其中至少约75wt%的生物馏分油组合物的沸点为约180-380℃,和其中生物馏分油组合物包含至少约50或40wt%的无氧烃。
在另一个实施方案中,本发明涉及一种生产可再生馏分油的方法,该方法包括:(a)将生物油分离为至少生物馏分油组合物,其中至少约75wt%的生物馏分油组合物的沸点为约180-380℃,其中生物油未预先经过脱氧加氢处理步骤;和(b)将至少一部分生物馏分油组合物与石油衍生馏分油范围的物流和具有表面活性剂性能的稳定添加剂合并,由此生成具有单一澄清相的可再生馏分油,其中可再生馏分油包含含量为约5-99wt%的石油衍生馏分油范围的物流、含量为至少约0.5wt%的生物馏分油组合物和含量为约0.5-25wt%的稳定添加剂。
在另一个实施方案中,本发明涉及一种总氧含量小于约15wt%的生物馏分油组合物,其中至少约75wt%的生物馏分油组合物的沸点为约180-380℃,和生物馏分油组合物包含至少约50或40wt%的无氧烃。
在另一个实施方案中,本发明涉及一种可再生馏分油组合物,该组合物包含含量为约5-99wt%的石油衍生馏分油范围的物流、含量为至少约0.5wt%的生物馏分油组合物和含量为约0.5-25wt%的具有表面活性剂性能的稳定添加剂。
附图说明
图1是本发明一个实施方案的生物质转化系统的示意图。
具体实施方式
图1描述了生物质转化系统10,它包括用于将生物油分离为多种馏分或燃料添加剂以及将生物馏分油组合物与石油衍生馏分油范围的物流共混作为共混原料或燃料添加剂以形成可再生馏分油的装置。
应当理解的是,图1中所示的生物质转化系统只是可以实现本发明的系统的一个例子。本发明可在多种其它系统中进行应用,这些系统均可以高效和有效地将生物油分离为可再生燃料和/或燃料添加剂。现对图1中所示的示例性生物质转化系统进行详细描述。
图1的生物质转化系统10包括生物质源12,用于供应生物质原料以供转化为生物油。生物质源12可以是例如漏斗、料仓、有轨车、路面拖车或任何其它可以保持或储存生物质的装置。由生物质源12供应的生物质可以是固体颗粒的形式。生物质颗粒可以是包含纤维素的纤维生物质材料。适合的含纤维素材料的例子包括藻类、造纸废料和/或棉籽绒。在一个实施方案中,生物质颗粒可包括木质纤维素材料。适合的木质纤维素材料的例子包括:林业废料,如木屑、锯屑、纸浆废料和树枝;农业废料,如玉米秸、麦秆和甘蔗渣;和/或能源作物,如桉树、柳枝稷和矮林。
如图1所示,可将来自生物质源12的固体生物质颗粒供应至生物质进料系统14。生物质进料系统14可以是任何能将固体生物质颗粒进料至生物质转化反应器16的系统。在生物质进料系统14中,生物质材料会经过若干预处理以利于后续的转化反应。该预处理可以包括干燥、焙烧、烘焙、脱矿物质、蒸汽喷发、机械搅拌和/或它们的任意组合。
在一个实施方案中,在将生物质引入生物质转化反应器16之前,可能需要在生物质进料系统14中将生物质与催化剂合并。替代地,可将催化剂直接引入生物质转化反应器16。催化剂可以是新鲜的和/或再生的催化剂。催化剂可以例如包括固体酸如沸石。适合的沸石的例子包括ZSM-5、丝光沸石、β沸石、镁碱沸石和Y沸石。此外,催化剂可以包括超酸。适合的超酸的例子包括氧化锆、氧化钛、氧化铝、氧化硅-氧化铝和/或粘土的磺化、磷酸盐化或氟化形式。在另一个实施方案中,催化剂可以包括固体碱。适合的固体碱的例子包括金属氧化物、金属氢氧化物和/或金属碳酸盐。特别适合的是碱金属、碱土金属、过渡金属和/或稀土金属的氧化物、氢氧化物和碳酸盐。其它适合的固体碱是层状双氢氧化物、混合的金属氧化物、水滑石、粘土和/或它们的组合。在另一个实施方案中,催化剂还可以包括氧化铝如α-氧化铝。
应当注意的是,固体生物质材料通常包含矿物质。可以认识到的是,这些矿物质中的一些如碳酸钾在生物质材料的转化中可以具有催化活性。
生物质进料系统14将生物质原料引入生物质转化反应器16。在生物质转化反应器16中,生物质经过转化反应,生成生物油。生物质转化反应器16可促进不同的化学转化反应,如快速热解、慢速热解、液化、气化或酶转化。生物质转化反应器16可以是例如流化床反应器、旋风反应器、烧蚀反应器或提升管反应器。
在一个实施方案中,生物质转化反应器16可以是提升管反应器和转化反应可以是快速热解。更具体地,快速热解可包括催化裂化。这里使用的“热解”是指通过在基本不含氧的气氛中加热原料引发的生物质的热化学转化。在一个实施方案中,在惰性气体如氮气、二氧化碳和/或蒸汽存在下进行热解。替代地,可在还原气体如氢气、一氧化碳、回收自生物质转化过程的不凝气和/或它们的任意组合存在下进行热解。
快速热解的特征在于生物质原料停留时间短和加热快。快速热解反应的停留时间可以是例如小于10秒、小于5秒或小于2秒。快速热解可在200-1000℃、250-800℃或300-600℃的温度下进行。
再参照图1,离开生物质转化反应器16的转化流出物18通常包含气体、蒸气和固体。如这里使用的,转化反应过程中产生的蒸气可互换地称为“生物油”,这是该蒸气冷凝为其液体状态时的常用名称。在本发明的一个实施方案中,在生物质转化反应器16中进行的转化反应生成生物油。该生物油的氧含量可以小于生物油的15、12、10或8wt%。氧含量也可以大于生物油的约0.5、1、3或5wt%。
当在生物质转化反应器16中进行快速热解时,转化流出物18通常包含炭、灰分和/或废催化剂的固体颗粒。可将转化流出物18引入固体分离器20。固体分离器20可以是任何能将固体与气体和蒸气分离的常规装置,例如旋风分离器或气体过滤器。固体分离器20从转化流出物18中脱除大部分固体(例如废催化剂、炭和/或热载体固体)。可将在固体分离器20中回收的固体颗粒22引入再生器24,典型地通过燃烧进行再生。再生后,可将至少一部分热的经再生固体经管线26直接引入生物质转化反应器16。替代地或另外地,可将热的经再生固体经管线28送至生物质进料系统14,用于在引入生物质转化反应器16之前与生物质进料合并。
然后,可将离开固体分离器20的基本上不含固体的流体物流30(也称为生物油)引入流体分离器32。在一个实施方案中,优选进入流体分离器32的生物油30未预先经过脱氧过程,例如加氢处理。流体分离器32可以是任何能将生物油30分离为至少轻质馏分34、生物馏分油馏分(组合物)36和重质馏分38的系统。用作流体分离器32的适合的系统包括例如通过分馏、加热蒸馏、萃取、膜分离、部分冷凝和/或非加热蒸馏进行分离的系统。在一些情况下,优选使用加热蒸馏进行分离,其中该加热蒸馏将生物油30的温度提高至100℃以上。如图1所示,可从流体分离器32中脱除不凝气40,和任选地经管线42将它循环至生物质转化反应器16,用作提升气体。
离开流体分离器32的轻质馏分34可具有与石油衍生汽油相当的沸程。离开流体分离器32的生物馏分油组合物36可具有与石油衍生馏分油相当的沸程。
生物馏分油组合物36的沸程可以是:至少75、85、95或100wt%的生物馏分油组合物36在约180-380℃、约190-370℃或约205-355℃的温度下沸腾。重质馏分38的沸程可以是:至少75、85、95或100wt%的重质馏分38在高于380℃、370℃或355℃的温度下沸腾。轻质馏分34的沸程可以是:至少75、85、95或100wt%的轻质馏分34在低于约205℃、190℃或180℃的温度下沸腾。
在一个实施方案中,将进入流体分离器32的生物油30的至少5、15、25或35wt%分离为生物馏分油组合物36。在另一个实施方案中,将进入流体分离器32的生物油30的至少10、20或30wt%分离为轻质馏分34,和将进行分离的生物油30的小于60wt%分离为重质馏分38。
生物馏分油馏分/组合物
生物馏分油组合物36的氧含量可以小于15、12、10、8wt%和/或大于约0.5、1或4wt%。生物馏分油组合物可以包含至少约40或50wt%的无氧烃,和可以含有小于约1或0.5wt%的羰基,和可以含有小于约0.5或0.2wt%的羧酸。
生物馏分油组合物可以含有小于约0.5或小于约0.2wt%的醛,和可以进一步包含约10-40wt%或约20-40wt%的含氧和碳的化合物。含氧和碳的化合物可选自酚、呋喃、酮、醛和它们的组合。
生物馏分油组合物的铜腐蚀测试值优选小于No.3。
可再生馏分油
如图1所示,生物质生产系统10可位于石油衍生馏分油源44附近或通过输送系统与其连通。石油衍生馏分油源44可以是例如石油炼厂、石油燃料储存设施和/或石油燃料输送系统。
可使用馏分油共混系统46将来自石油衍生馏分油源44的石油衍生馏分油范围的物流48与至少一部分生物馏分油组合物36和稳定添加剂50合并以生成具有单一澄清相的可再生馏分油组合物52,其中石油衍生馏分油范围的物流48每分子可含有12-25个碳原子。
可再生馏分油组合物可包含:含量为至少5、15或25wt%和/或至多99、98或96wt%的石油衍生馏分油范围的物流48;含量为至少0.5、2、5、25或60wt%的生物馏分油组合物36;和含量为约0.5-25wt%的具有表面活性剂性能的稳定添加剂。
稳定添加剂可包括选自如下的材料:1)亲水亲油平衡值(HLB)为至多8、7或6和/或至少2或3的非离子嵌段共聚物;2)HLB为至多8、7或6和/或至少2或3的非离子均聚物;3)平均HLB为至多8、7或6和/或至少2或3的非离子嵌段共聚物和非离子均聚物的混合物;4)HLB为至多8、7或6和/或至少2或3的非离子表面活性剂;5)脂肪酸甲基酯(FAME);或6)它们的组合。稳定添加剂的例子包括但不限于:Hypermer系列聚合物、Brij系列表面活性剂、异硬脂酸丙二醇酯、Span系列表面活性剂、硬脂酸乙二醇酯、倍半油酸脱水山梨醇酯、硬脂酸甘油酯、卵磷脂系列表面活性剂、油酸脱水山梨醇酯、单硬脂酸脱水山梨醇酯NF、硬脂酸脱水山梨醇酯、异硬脂酸脱水山梨醇、硬脂基聚氧乙烯(2)醚、油基聚氧乙烯(2)醚、月桂酸甘油酯、十六烷基聚氧乙烯(2)醚、PEG系列聚合物表面活性剂、二多羟基硬脂酸酯、硬脂酸甘油酯SE、甲基葡萄糖倍半硬脂酸酯、Atsurf系列表面活性剂和它们的组合。
在其它选择中,石油衍生馏分油范围的物流可以选自常规馏分油、低硫馏分油、经加氢处理的轻质循环油、经加氢处理的直馏瓦斯油、超低硫馏分油、经精炼处理的中间馏分油或它们的组合。
在使用的稳定添加剂包括非离子表面活性剂、非离子嵌段共聚物、非离子均聚物或非离子嵌段共聚物和非离子均聚物的混合物的情况下,为便于处理,优选同时或顺序将稳定添加剂和生物馏分油组合物加入石油衍生馏分油范围的物流,由此形成可再生馏分油。
在稳定添加剂包括FAME的情况下,已经发现通过将生物馏分油组合物与稳定添加剂合并、然后再将这两种组分与石油衍生馏分油范围的物流合并、由此形成可再生馏分油,可以获得明显的操作上的便利。
实施例
实施例1
在反应器出口温度为约650℃下操作的提升管反应器中,在催化剂存在下通过热解转化南方黄松木颗粒而生成低氧生物油。得到的生物油的氧含量为约12wt%,和经过蒸馏得到大于25wt%的沸程低于约345℃的生物馏分油组合物。生物馏分油组合物的组成示于下表1中。
表1
从数据可以看出,生物馏分油组合物质量高、氧含量低、未检出羧酸、和环状化合物/芳族化合物含量大。
实施例2
将一定量的HypermerB241聚合物与商购的超低硫柴油(ULSD)共混以形成第一混合物,然后将它与一定量实施例1的生物馏分油组合物合并以形成可再生馏分油共混物,该共混物中含有97wt%的ULSD、1wt%的HypermerB241和2wt%的生物馏分油。使用超声均化器混合后,可再生馏分油共混物为单一澄清相。
实施例3
将不同量的FAME与不同量实施例1的生物馏分油组合物共混以形成混合物,然后将它与不同量的ULSD合并以形成可再生馏分油共混物,用超声均化器混合所述共混物。全部共混物所得到的单一澄清相示于下表2中。
表2
实施例4
将不同量实施例1的生物馏分油组合物与ULSD共混,使用1wt%的HypermerB246聚合物材料形成含2%生物馏分油(BD)的共混物,HLB值为6;和使用2.5wt%的FAME(获自Houston,TX的HoustonBiodiesel公司)形成含40%生物馏分油(BD)的另一共混物。测试ULSD和各种共混物的多种性质/组分。该测试的结果显示在下表3中。表3还包括两种馏分油石油产物柴油#2S500(D2S500)和燃料油#2(FO#2)的那些性质的规定值。观察到得到的共混物变得澄清和稳定,共混物符合常规馏分油的规格。
表3
从上面表3可以看出,通过将生物馏分油、添加剂和ULSD共混而制成的可再生馏分油的性质符合馏分油燃料的规格。含2wt%生物柴油的可再生馏分油满足柴油#2-S500的规格,而含40%生物柴油的可再生馏分油满足燃料油#2规格(对于40%BD共混物来说,密度和兰氏残碳除外)。
上述本发明的优选形式仅用于举例说明,不应当用于限制性地解释本发明的范围。本领域技术人员可以容易地对上述示例性实施方案做出调整,而不背离本发明的精神。
发明人意图依靠等同原则来确定和评估本发明的合理公平的范围,该范围涉及虽处于如下权利要求书所述发明的字面范围之外但实质上并不与之背离的任何方法和系统。
Claims (23)
1.一种生产可再生馏分油的方法,该方法包括:
(a)将生物油分离为至少生物馏分油馏分,其中至少75wt%的所述生物馏分油馏分的沸点为180-380℃,其中所述生物油未预先经过脱氧加氢处理步骤;和
(b)将至少一部分所述生物馏分油馏分与石油衍生馏分油范围的物流和具有表面活性剂性能的稳定添加剂合并,由此生成具有单一澄清相的可再生馏分油,其中所述可再生馏分油包含含量为5-99wt%的所述石油衍生馏分油范围的物流、含量为至少0.5wt%的所述生物馏分油馏分和含量为0.5-25wt%的所述稳定添加剂。
2.权利要求1的方法,其中所述稳定添加剂包括选自如下的材料:1)亲水亲油平衡值(HLB)为至多8的非离子嵌段共聚物;2)HLB为至多8的非离子均聚物;3)平均HLB为至多8的非离子嵌段共聚物和非离子均聚物的混合物;4)HLB为至多8的非离子表面活性剂;5)脂肪酸甲基酯(FAME);或6)它们的组合。
3.权利要求2的方法,其中所述非离子嵌段共聚物、所述非离子均聚物、所述非离子嵌段共聚物和非离子均聚物的混合物以及所述非离子表面活性剂的HLB值均为至少2。
4.权利要求1的方法,其中所述稳定添加剂是FAME。
5.权利要求4的方法,其中所述可再生馏分油包含含量为至少0.5wt%的所述生物馏分油馏分。
6.权利要求4的方法,其中所述可再生馏分油包含含量为至少5wt%的所述生物馏分油馏分。
7.权利要求1的方法,其中所述石油衍生馏分油范围的物流选自常规馏分油、低硫馏分油、经加氢处理的轻质循环油、经加氢处理的直馏瓦斯油、超低硫馏分油、经精炼处理的中间馏分油或它们的组合。
8.权利要求1的方法,其中所述石油衍生馏分油范围的物流包含每分子含有12-25个碳原子的烃。
9.权利要求2的方法,其中所述稳定添加剂包括所述非离子嵌段共聚物、所述非离子均聚物、所述非离子表面活性剂或它们的混合物;和其中同时或顺序将所述稳定添加剂和所述生物馏分油馏分加入所述石油衍生馏分油范围的物流,由此形成可再生馏分油。
10.权利要求2的方法,其中所述稳定添加剂包括FAME;和其中将所述生物馏分油馏分与所述稳定添加剂合并,然后再与所述石油衍生馏分油范围的物流合并,由此形成可再生馏分油。
11.权利要求1的方法,其中将经过步骤(a)分离的所述生物油的至少5wt%分离为所述生物馏分油馏分。
12.权利要求1的方法,其中步骤(a)的分离通过分馏完成。
13.权利要求1的方法,其中所述生物油得自催化剂存在下生物质的热化学转化。
14.权利要求1的方法,其中所述生物油的总氧含量小于15wt%。
15.一种可再生馏分油组合物,该组合物包含含量为5-99wt%的石油衍生馏分油范围的物流、含量为至少0.5wt%的生物馏分油馏分和含量为0.5-25wt%的具有表面活性剂性能的稳定添加剂,其中从生物油中分离所述生物馏分油馏分,其中至少75wt%的所述生物馏分油馏分的沸点为180-380℃,和其中在分离所述生物馏分油馏分之前所述生物油未预先经过脱氧加氢处理步骤。
16.权利要求15的可再生馏分油组合物,其中所述稳定添加剂包括选自如下的材料:1)HLB为至多8的非离子嵌段共聚物;2)HLB为至多8的非离子均聚物;3)平均HLB为至多8的非离子嵌段共聚物和非离子均聚物的混合物;4)HLB为至多8的非离子表面活性剂;5)FAME;或6)它们的组合。
17.权利要求16的可再生馏分油组合物,其中所述非离子嵌段共聚物、所述非离子均聚物、所述非离子嵌段共聚物和非离子均聚物的混合物以及所述非离子表面活性剂的HLB值均为至少2。
18.权利要求16的可再生馏分油组合物,其中所述稳定添加剂是FAME。
19.权利要求18的可再生馏分油组合物,其中所述可再生馏分油组合物包含含量为至少25wt%的所述生物馏分油馏分。
20.权利要求18的可再生馏分油组合物,其中所述可再生馏分油组合物包含含量为至少0.5wt%的所述生物馏分油馏分。
21.权利要求15的可再生馏分油组合物,其中所述石油衍生馏分油范围的物流选自常规馏分油、低硫馏分油、经加氢处理的轻质循环油、经加氢处理的直馏瓦斯油、超低硫馏分油、经精炼处理的中间馏分油或它们的组合。
22.权利要求15的可再生馏分油组合物,其中所述石油衍生馏分油范围的物流包含每分子含有12-25个碳原子的烃。
23.权利要求15的可再生馏分油组合物,其中所述生物油得自催化剂存在下生物质的热化学转化。
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CN103189479A (zh) | 2013-07-03 |
US20120266526A1 (en) | 2012-10-25 |
EP2633006A1 (en) | 2013-09-04 |
US8454712B2 (en) | 2013-06-04 |
CA2811646A1 (en) | 2012-05-03 |
EP2633006B1 (en) | 2019-05-22 |
EP2633006A4 (en) | 2014-08-13 |
CA2811646C (en) | 2021-01-19 |
US8377152B2 (en) | 2013-02-19 |
US20120260564A1 (en) | 2012-10-18 |
US20120017492A1 (en) | 2012-01-26 |
US8506658B2 (en) | 2013-08-13 |
BR112013009843A2 (pt) | 2016-07-26 |
WO2012057988A1 (en) | 2012-05-03 |
DK2633006T3 (da) | 2019-08-19 |
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