等离子体处理稠油的机理与研究
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摘要
随着轻质原油的不断减少以及人们对石油资源需求的不断增加,迫使人们纷纷把目光转向资源量相对丰富的重质原油的开发和利用。重质原油的高粘度特性使其在井筒举升和集输中不易流动,其较高的金属杂质含量常常使催化加工中催化剂中毒失活。为了使重油轻质化,实现重油的高效开发和利用,人们不断地寻找新技术,等离子体技术就是其中之一。
介质阻挡放电等离子体处理重油,较传统的技术有许多优势,但是目前该技术还处于实验室研究阶段。本文在国内外研究工作的基础上,分别作了等离子体处理柴油和重油的研究,并对反应机理了做了讨论。为了研究的简便性,首先研究了原油的馏分产品柴油在等离子体作用下的变化情况,柴油经空气DBD等离子体处理后,颜色加深,有刺激性气味气体生成,阻挡介质石英片上有胶状物产生,柴油的粘度、元素组成、红外光谱和表面张力都发生了变化;经氩气DBD等离子体处理后,气相色谱分析有氢气、低分子烷烃和少量的烯烃生成。在柴油实验研究的基础上,对柴油的裂解机理作了分析,选取正庚烷作为柴油的模型化合物,设计了正庚烷在高能电子作用下的初始裂解反应,共包括13个反应,并计算了各反应的反应速率,拟合得到了Arrhenius公式的三参数。最后,对稠油进行了等离子体处理,空气等离子体处理稠油有难闻气体和胶状物生成,稠油的粘度、四组分和红外光谱都发生了变化,机理分析显示主要是氧化反应所致;氩气等离子体处理稠油后有气体生成,产物组分包括氢气、低分子烷烃和少量烯烃,机理分析认为主要是烷基链的断裂反应。通过实验和理论研究发现,使用介质阻挡放电等离子体可以使柴油、稠油在室温条件下发生化学反应,裂解生成氢气和低碳烃类,剩余油粘度升高,有待作进一步的研究。
With decrease of light crude oil and increase of the demand for crude oil, development and utilization of heavy oil is becoming more and more important. The characteristics of high viscosity of heavy oil made it difficult in the wellbore lifting, gathering and transporting pipeline, its high content of metal impurities always cause the catalyst poisoning and deactivation in the heavy oil process. In order to convert the heavy oil to light and to achieve efficient exploitation and utilization of heavy oil, people are making efforts to looking for new technologies; the plasma technology is one of them.
Using dielectric barrier discharge plasma updating heavy oil has many advantages, but currently this technology is still in the laboratory research stage. Based on situation of the present developing researches at home and abroad, this paper studys the diesel and heavy oil treated by DBD plasma, discusses the crack mechanism of diesel and heavy oil. Simply, we first treated the diesel using DBD plasma, in the air DBD plasma process, The color changes of diesel, the production of gas with pungent odor and the appearance of jelly on the quartz medium plate were observed, while viscosity, elemental composition, infrared spectroscopy and surface tension of diesel were changing; in the argon DBD plasma process, the result of gas chromatography of gas products showed that it contains hydrogen, low molecular weight alkanes and a small amount of alkenes. Based on experiment, n-heptane was selected as model compoun, and its cracking mechanism contains 13 reactions induced by incident electron was designed; reaction rate of each reaction was calculated and three parameter in Arrhenius formula was obtained. Finally, heavy oil was treated, in the air DBD plasma process, also gas and jelly product were abserved, the viscosity, infrared spectroscopy and SARA were changing, mechanism analysis showed they were the result of oxidizing reaction. In the argon DBD plasma, GC result showed hydrogen, low molecular weight alkanes and a small amount of alkenes, we considered it is the crack result of alkyl chain. Experimental and theoretical study found that both diesel and heavy oil could be cracked by DBD plasma, hydrogen and C1~C5 hydrocarbons were produced, but the oil viscosity increased after the DBD plasma treatment, further study has to be done.
介质阻挡放电等离子体处理重油,较传统的技术有许多优势,但是目前该技术还处于实验室研究阶段。本文在国内外研究工作的基础上,分别作了等离子体处理柴油和重油的研究,并对反应机理了做了讨论。为了研究的简便性,首先研究了原油的馏分产品柴油在等离子体作用下的变化情况,柴油经空气DBD等离子体处理后,颜色加深,有刺激性气味气体生成,阻挡介质石英片上有胶状物产生,柴油的粘度、元素组成、红外光谱和表面张力都发生了变化;经氩气DBD等离子体处理后,气相色谱分析有氢气、低分子烷烃和少量的烯烃生成。在柴油实验研究的基础上,对柴油的裂解机理作了分析,选取正庚烷作为柴油的模型化合物,设计了正庚烷在高能电子作用下的初始裂解反应,共包括13个反应,并计算了各反应的反应速率,拟合得到了Arrhenius公式的三参数。最后,对稠油进行了等离子体处理,空气等离子体处理稠油有难闻气体和胶状物生成,稠油的粘度、四组分和红外光谱都发生了变化,机理分析显示主要是氧化反应所致;氩气等离子体处理稠油后有气体生成,产物组分包括氢气、低分子烷烃和少量烯烃,机理分析认为主要是烷基链的断裂反应。通过实验和理论研究发现,使用介质阻挡放电等离子体可以使柴油、稠油在室温条件下发生化学反应,裂解生成氢气和低碳烃类,剩余油粘度升高,有待作进一步的研究。
With decrease of light crude oil and increase of the demand for crude oil, development and utilization of heavy oil is becoming more and more important. The characteristics of high viscosity of heavy oil made it difficult in the wellbore lifting, gathering and transporting pipeline, its high content of metal impurities always cause the catalyst poisoning and deactivation in the heavy oil process. In order to convert the heavy oil to light and to achieve efficient exploitation and utilization of heavy oil, people are making efforts to looking for new technologies; the plasma technology is one of them.
Using dielectric barrier discharge plasma updating heavy oil has many advantages, but currently this technology is still in the laboratory research stage. Based on situation of the present developing researches at home and abroad, this paper studys the diesel and heavy oil treated by DBD plasma, discusses the crack mechanism of diesel and heavy oil. Simply, we first treated the diesel using DBD plasma, in the air DBD plasma process, The color changes of diesel, the production of gas with pungent odor and the appearance of jelly on the quartz medium plate were observed, while viscosity, elemental composition, infrared spectroscopy and surface tension of diesel were changing; in the argon DBD plasma process, the result of gas chromatography of gas products showed that it contains hydrogen, low molecular weight alkanes and a small amount of alkenes. Based on experiment, n-heptane was selected as model compoun, and its cracking mechanism contains 13 reactions induced by incident electron was designed; reaction rate of each reaction was calculated and three parameter in Arrhenius formula was obtained. Finally, heavy oil was treated, in the air DBD plasma process, also gas and jelly product were abserved, the viscosity, infrared spectroscopy and SARA were changing, mechanism analysis showed they were the result of oxidizing reaction. In the argon DBD plasma, GC result showed hydrogen, low molecular weight alkanes and a small amount of alkenes, we considered it is the crack result of alkyl chain. Experimental and theoretical study found that both diesel and heavy oil could be cracked by DBD plasma, hydrogen and C1~C5 hydrocarbons were produced, but the oil viscosity increased after the DBD plasma treatment, further study has to be done.
引文
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[8] G. S. Kovener. Use of an rf plasma for the thermal pyrolysis of CH4 and heavy oils[A]. ISPC-6 Montreal, 1983: 258-263.
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[15] Peter C. Kong. Method for cracking hydrocarbon compositions using a submerged reactive plasma system[P]. US Patent:5626726, 1997-5-6.
[16] Graciela Prieto, Mamoru Okumoto. Reforming of Heavy Oil Using Nonthermal Plasma[J]. IEEE transactions on industry applications, 2001, 37(5): 1464-1467.
[17] Graciela Prieto, Mamoru Okumoto. A Plate-to-Plate Plasma Reactor as a Fuel Processor for Hydrogen-Rich Gas Production. 2001,1099-1102
[18] Maurice G. Fey, Plum Borough, Pa. Arc Heater Apparatus for Producing Acetylene From Heavy Hydrocarbons[P]. USA: 4,105,888, 1978(8).
[19] Jacques Amouroux, Mehrdad Nikravech. Process For The Hydrocracking of A Hydrocarbon Feedstock And Hydrocracking Plant For Carrying[P]. USA: 4,941,965, 1990(7).
[20] Peter C. Kong, Paul A. Lessing. Method and Apparatus For Producing Oxygenates From Hydrocarbons[P]. USA: 5,427,747, 1995(6).
[21] Peter C. Kong, Lee O. Nelson. Nonthermal Plasma Systems and Methods For Natural Gas and Heavy Hydrocarbon Co-conversion[P]. USA: 6,896,854 B2, 2005(5).
[22] Shyam V. Dighe, Mark Anthony Montemurro. Martorell. System and Process For Upgrading Heavy Hydrocarbons[P]. USA: 2008/0299019 A1, 2008(4).
[23] Peter C. Kong, Lee O. Nelson, Brent A. Detering. Methods For Natural Gas and Heavy Hydrocarbon Co-conversion[P]. USA: 7,494,574 B2, 2009(2).
[24] R. W. Grimes, Francis. P. Miknis. Preliminary evaluation of a process using plasma reactions to desulfurize heavy oil[R]. Laramie: 1997.
[25] F.P.Miknis Fossil fuel and hydrocarbon conversion using hydrogen-rich plasmas[R]. Laramie: 1994-1995.
[26] Langmuir, I. Proceedings of the National Academy of Sciences of the United States of America[J]. 1928, 14(8): 627.
[27]许根慧,姜恩永等.等离子体技术与应用[M].北京:化学工业出版社, 2006: 1-2.
[28]博伊德等.等离子体动力学[M].戴世强等译.北京:科学出版社, 1977.
[29] Fridman A, Chirokov A and Gutsol A. Non-themmal atmospheric pressure discharge,J.Phys. D:Appl.Phys. 2005, 38: 224.
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