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铁系油溶性催化剂在稠油水热裂解上的应用分析.pdf

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摘要摘要随着世界上常规原油的不断消耗以及近期油价的不断攀升,储量巨大的稠油在石油资源的开采所占的比例也越来越大。常规的稠油开采方法主要是蒸汽吞吐和蒸汽驱,但是由于稠油所具有的高黏度、高密度等特点造成了开采、集输以及地面炼制方面的困难。在长期的石油工业研究中,人们发现了水热裂解反应,即存在于热力采油中的化学变化使稠油黏度降低的现象,并提出利用催化剂促进水热裂解反应程度的新思路。本文以胜利油田稠油为研究原料,考察两种铁系油溶性水热裂解催化剂十二烷基苯磺酸铁和乙酰丙酮铁在160.240℃之间的降黏效果,在24 h的反应时间下,考察反应温度,油水比和催化剂投药量对反应结果的影响,此外利用甲酸作为供氢剂考察了乙酰丙酮铁和甲酸共同作用催化水热裂解反应的影响。实验结果表明在200℃,油水质量比为73,催化剂投药量为稠油质量O.5%的时候,十二烷基苯磺酸铁对胜利撑1稠油的催化降黏率达到了71.52%;在240℃,油水质量比为73,催化剂投药量为稠油质量0.3%的时候乙酰丙酮铁对胜利舵稠油的催化降黏率达到了68.18%而在加入3%的甲酸后,在各个温度点下铊稠油的降黏率相对于未加入甲酸时相比都有部分提升。通过对反应后稠油族组分的分离,对反应前后稠油S肌~饱和烃、芳香烃、胶质、沥青质含量进行了对比,对重质组分进行了元素分析、红外分析和核磁氢谱分析并与反应前胶质、沥青质进行了相应比较。分析结果显示反应后SARA族中重质组分含量大幅降低而轻质组分则相应增加,元素分析等结果也显示在反应后重质组分中的硫、氮原子减少,氢碳比增加,原油饱和度增加,化合物结构发生较大的变化,说明在两种催化剂的作用下,稠油都发生了水热裂解化学变化,使得稠油中重质组分向轻质组分的转换,最终导致稠油黏度的降低而改善其流动性,而甲酸的加入则为反应提供足够的氢源,进一步降低反应后稠油的黏度。关键词稠油水热裂解降黏铁系催化剂AbstractWim the increasing consumption and rising price of crude oil,recovery of heavyoils from the ation becomes significant due to its large proportion in the total oilstorage.Nowadays,the recovery ofheavy oils is mainly by means ofthermal recovery,such as steam huff and puif,steam flood.But with the features as both hi【gh viscosityand high density,there are enormous difficulties in recovery,delivery and refine ofheavy oils.During the longterm application research,scientists found some chemicalchanges of heavy oils while these thermal recovery s were applied,and thereduction of viscosity were observed.ncy called it aquathermolysis,and later lots ofefforts have been carried out to use catalysts to promote this effect.In this article,twooibsoluble iron-based catalysts,ferric dodccylbenzenesulphonate and ferricacetylacetonate were prepared to uate the catalytic perance inaquathermolysis of Shengli heavy oils.Under the reaction time of 24 h,the optimumreaction temperature,mass ratio of oil to water and catalyst dosage were obtained.Inaddition,ic acid was uated as a hydrogen donor tO enhance the reduction ofviscosity.The experimental results indicated that the reduction of viscosity Can be up to7 1.52%under the conditionsreaction temperature is 200℃,mass ratio of oil towater is 73 and catalyst dosage is O.5%.In another ca∞,the reduction of viscosityCan be up to 68.1 8%under these conditionsreaction temperature is 240℃,massratio of oil to water is 73 and catalyst dosage is 0.3%.Moreover,the reduction ofviscosity at each temperature points w饿all further promoted while ic acid Wasadded as a hydrogen donor.ARer the reaction,SARA components were separated,the content of light andheavy components were measured.Results indicated that heavy componentsⅡAbstractdecreased and light components increased obviously in comparison with those beforethe reaction·Furthermore,asphaltene and resin were analyzed by FT-IR,elementaryanalysis and 1H-NMR.It is found H/Cmolar ratioincreased,and content of sulfurand nitrogen decreased after the reaction with the two catalysts above.Meanwhile,structure of the heavy components engaged in big changes.All these resultsdemonstrated that the two catalysts Can reduce the viscosity to a big extent andimprove the flow properties of the heavy oils.Furthermore,in contrast to the rcactioncatalyzed by ferric acetylacetonate alone,addition of ic acid Can further improveeffects of the aquathermolysis.Key wordsheavy oil;aquathermolysis;viscosity reduction;iron-based catalystsIll耳录目 录摘|要........。.....................................。....。.........。......。.....。............IAbstract.........................................................................................II第一章文献综述.Ⅳ1.1稠油的基本概念及性质 l1.1.1稠油的定义及分类标准l1.1.2稠油的组成和特点.21.2影响稠油黏度的因素 31.2.1胶质和沥青质含量对稠油黏度的影响31.2.2胶质和沥青质结构对稠油黏度的影响.41.2.3石蜡对稠油黏度的影响51.3稠油开采方法 61.3.1掺稀油降黏采油61.3.2蒸汽吞吐。71.3.3蒸汽驱.71.3.4火烧油层.81.3.5表面活性剂驱81.3.6油溶性降黏采油.91.3.7加碱降黏采油.91.3.8微生物降黏采油10水热裂解催化降黏开采 1l1.4.1水热裂解可行性分析.1l1.4.2催化水热裂解l 21.4.3水热裂解研究进展14I目录1.5本课题的研究内容.1.6本课题的研究意义 16第二章实验部分172.1实验原料2.2实验试剂及仪器172.2.1 实验仪器。1 72.2.2实验试剂.....1 82.3稠油性质分析方法2.3.1稠油黏度测定192.3.2稠油中SARA族的分离。202.4催化剂的选择、制备及评价方法 ..212.4.1十二烷基苯磺酸铁的制备..222.4.2催化剂的评价方法242.5 FT-IR分析.2.6元素分析。2.7核磁氢谱分析..262727第三章十二烷基苯磺酸铁降黏效果及分析..283.1十二烷基苯磺酸铁对稠油催化水热裂解降黏的影响.283.1.1 反应温度对稠油催化水热裂解反应的影响。283.1.2油水比对稠油催化水热裂解反应的影响。293.1.3催化剂投药量对稠油催化水热裂解反应的影响303.2十二烷基苯磺酸铁催化水热裂解降黏分析.3.2.1 SARA族组成含量变化分析323.2.2反应前后沥青胶质元素分析.323.2.3反应前后沥青质、胶质瓜分析.333.2.4反应前后沥青质、胶质核磁共振分析。343.3本章小结Ⅱ目录第四章 乙酰丙酮铁降黏效果及分析.414.1 乙酰丙酮铁对稠油催化水热裂解降黏的影响. 414.1.1 反应温度对稠油催化水热裂解反应的影响..414.1.2油水比对稠油催化水热裂解反应的影响424.1.3催化剂投药量对稠油催化水热裂解反应的影响..434.2乙酰丙酮铁催化水热裂解降黏分析4.2.1 S肌~族组成含量变化分析444.2.2反应前后沥青胶质元素分析。454.2.3反应前后沥青质、胶质瓜分析.464.2.4反应前后沥青质、胶质核磁共振分析。474.3本章小结第五章 甲酸对乙酰丙酮铁催化水热裂解的影响.52 ’5.1 甲酸对乙酰丙酮铁的催化水热裂解影响5.2甲酸作为供氢剂协同乙酰丙酮铁降黏分析53545.2.1 SARA族组成含量变化分析545.2.2反应前后沥青胶质元素分析555.2.3反应前后沥青质、胶质瓜分析565.2.4反应后沥青质、胶质核磁共振分析。575.3本章小结第六章总结与建议。。..606.1总结6.2建议参考文献..6062..........................................................63攻读硕士学位期间发表的成果。致谢.Ⅲ6768仉lble ofContentsTable of ContentsAbstract in Chinese.....................................................................IAbstract in English.........................................................................IIChapter 1 Literatures ReviewⅣ1.1 Basic Knowledge and Characteristics of Heavy Oils....1.1.1 Definition and Classifcation of Heavy Oils...11.1.2 Composition and Characteristics ofHeavy Oils..21.2 Effect of Different Factors on Viscosity 31.2.1 Effect of Resin and Asphaltene Content on Viscosity..31.2.2 Effect of Resin and Asphaltene Structure on Viscosity41.2.3 Effect of Petroleum Wax on Viscosity..51.3 s of Heavy oiIs Recovery 61.3.1 Light Oil Blending..61.3.2 Steam}Iu行and Pu正。71.3.3 Steam Stimulation71.3.4 In.Situ Combustion.81.3.5 Surfactant Flooding....81.3.6 Oilsoluble Viscosity-reducing Agent Flooding..91.3.7 Alkaline Flooding...91.3.8 Microbial Enhanced Oil Recovery...101.4 Catalytic Auqthermoysls for Heavy oils Recovery ll1.4.1 Feasibility ofAquthermolysis.1 l1.4.2 Technologies of Catalytic Auqthermolysis..121.4.3 Research on Catalytic Auathermolysis..141.5 Major Contents of This Thesis1.6 Purpose of This ThesisChapter 2 Materials and s................IV...........17
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