煤裂解制乙炔过程颗粒尺度传递和反应行为研究
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摘要
热等离子体裂解煤制乙炔过程为煤的直接化工利用提供了一条有前景的、清洁转化途径。该过程是高温毫秒级超短接触反应过程,但目前的检测手段还无法探测等离子体下毫秒级的条件下颗粒的反应行为,使得煤的毫秒级超高温裂解过程的基础研究极为匮乏。另一方面,由于该过程还未成功大规模工业化,对这一过程的经济性分析也比较欠缺。
本文主要在煤常规物理及热解特性、煤高温裂解过程中颗粒尺度传递和反应行为模拟以及技术经济分析三个方面开展了工作。
通过对原煤、常规热解后残渣和等离子体裂解后残渣的对比,发现煤粉在等离子体中裂解首先经历了与常规热解类似的脱挥发分过程,但这一过程持续时间非常短,在超过2000 K的环境流体作用下,煤中更多的有机物质参与了裂解反应,提高了气相产物中C、H元素的比例,有利于生成更多的目标产物乙炔。这说明煤粉经历的温度范围及脱挥发分过程直接决定了反应器的乙炔产率。
结合该过程超高温、超短接触的特征,通过建立描述单颗粒煤粉高温快速裂解过程的机理模型,分别考察了在恒温环境流体和气固传热耦合条件下的颗粒尺度传递和反应行为,指出颗粒自身有限导热及挥发分逸出所产生的两种传热阻力对煤脱挥发分过程的模型和模拟中都是不可忽略的。研究表明,针对毫秒级煤裂解过程,大于100μm的煤粉,平均温度低于2000 K的等离子体气体,过高或过小的煤/氢进料比难于实现满意的脱挥发分行为。
基于元素守恒原则,对中试系统进行物料和能量衡算,指出反应器性能主要取决于气固混合效率、煤/氢进料比及反应停留时间。若进一步实施能量综合利用方案,系统的能量利用效率会大幅提高。在此基础上,对煤制乙炔过程进行了乙炔生产成本核算,原料煤价格和电价是制约乙炔成本中最主要的部分,通过进一步改善反应器性能,提高气相产品总流量和乙炔浓度都将降低乙炔生产成本。
Coal pyrolysis to acetylene in thermal plasma provides a direct route to make chemicals from coal resources. This process is operated under high temperature and has contact time of milliseconds scale. Direct measurements inside the reactor are hardly implemented, which obstruct further studies of this kind of process. On the other hand, since the process has not been successfully industrialized in large scale, the economic analysis of it is also insufficient.
In this work, the raw coal and residues after the decomposition and the plasma pyrolysis was analyzed. The results implied that ultrahigh temperature (>2000 K) broke more chemical bonds and formed more hydrocarbon than that of the decomposition process, and increased the ratio of C and H in the gas phase, which facilitated the generation of acetylene. The temperature of the coal and the depth of devolatilization would determine the yield of acetylene.
A mechanism model incorporating the heat conduction in solid materials, diffusion of released volatile gases and reactions was proposed for a deep understanding of the heat transport inside a coal particle under the extreme environmental conditions, such as temperatures higher than 2,000 K and reaction time in milliseconds. Thermal balance between coal particles and the hot carrier gas was established. The predicted yield of volatiles considering the mechanism of the two resistances agreed reasonably with the experimental data under different operating conditions, and this effect became more evident for larger particles. It can be concluded that the proposed heat transport mechanism inside coal particles worked well in understanding the coal pyrolysis process at ultra-high temperatures. Limited by the milliseconds process of the coal pyrolysis, particles of size greater than 100μm or heating fluid of temperature lower than 2000 K is not recommended in the practical application due to the slow release of volatiles in coals.
Furthermore, the materials balance and energy balance of the process was investigated systematically based on element balance. It is concluded that the overall plasma reactor performance was dominated by the gas-solid mixing efficiency, coal-hydrogen feeding rate and the residence time. Based on these constrains, the economic analysis of acetylene production indicated that the costs of raw coal and power were the main parts. The optimal utilization of energy and material-flows in the system can be of great significance to ensure the economic feasibility.
本文主要在煤常规物理及热解特性、煤高温裂解过程中颗粒尺度传递和反应行为模拟以及技术经济分析三个方面开展了工作。
通过对原煤、常规热解后残渣和等离子体裂解后残渣的对比,发现煤粉在等离子体中裂解首先经历了与常规热解类似的脱挥发分过程,但这一过程持续时间非常短,在超过2000 K的环境流体作用下,煤中更多的有机物质参与了裂解反应,提高了气相产物中C、H元素的比例,有利于生成更多的目标产物乙炔。这说明煤粉经历的温度范围及脱挥发分过程直接决定了反应器的乙炔产率。
结合该过程超高温、超短接触的特征,通过建立描述单颗粒煤粉高温快速裂解过程的机理模型,分别考察了在恒温环境流体和气固传热耦合条件下的颗粒尺度传递和反应行为,指出颗粒自身有限导热及挥发分逸出所产生的两种传热阻力对煤脱挥发分过程的模型和模拟中都是不可忽略的。研究表明,针对毫秒级煤裂解过程,大于100μm的煤粉,平均温度低于2000 K的等离子体气体,过高或过小的煤/氢进料比难于实现满意的脱挥发分行为。
基于元素守恒原则,对中试系统进行物料和能量衡算,指出反应器性能主要取决于气固混合效率、煤/氢进料比及反应停留时间。若进一步实施能量综合利用方案,系统的能量利用效率会大幅提高。在此基础上,对煤制乙炔过程进行了乙炔生产成本核算,原料煤价格和电价是制约乙炔成本中最主要的部分,通过进一步改善反应器性能,提高气相产品总流量和乙炔浓度都将降低乙炔生产成本。
Coal pyrolysis to acetylene in thermal plasma provides a direct route to make chemicals from coal resources. This process is operated under high temperature and has contact time of milliseconds scale. Direct measurements inside the reactor are hardly implemented, which obstruct further studies of this kind of process. On the other hand, since the process has not been successfully industrialized in large scale, the economic analysis of it is also insufficient.
In this work, the raw coal and residues after the decomposition and the plasma pyrolysis was analyzed. The results implied that ultrahigh temperature (>2000 K) broke more chemical bonds and formed more hydrocarbon than that of the decomposition process, and increased the ratio of C and H in the gas phase, which facilitated the generation of acetylene. The temperature of the coal and the depth of devolatilization would determine the yield of acetylene.
A mechanism model incorporating the heat conduction in solid materials, diffusion of released volatile gases and reactions was proposed for a deep understanding of the heat transport inside a coal particle under the extreme environmental conditions, such as temperatures higher than 2,000 K and reaction time in milliseconds. Thermal balance between coal particles and the hot carrier gas was established. The predicted yield of volatiles considering the mechanism of the two resistances agreed reasonably with the experimental data under different operating conditions, and this effect became more evident for larger particles. It can be concluded that the proposed heat transport mechanism inside coal particles worked well in understanding the coal pyrolysis process at ultra-high temperatures. Limited by the milliseconds process of the coal pyrolysis, particles of size greater than 100μm or heating fluid of temperature lower than 2000 K is not recommended in the practical application due to the slow release of volatiles in coals.
Furthermore, the materials balance and energy balance of the process was investigated systematically based on element balance. It is concluded that the overall plasma reactor performance was dominated by the gas-solid mixing efficiency, coal-hydrogen feeding rate and the residence time. Based on these constrains, the economic analysis of acetylene production indicated that the costs of raw coal and power were the main parts. The optimal utilization of energy and material-flows in the system can be of great significance to ensure the economic feasibility.
引文
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[2] Bond R L, Galbraith I F, Ladner W R, McConnell G I T. Production of acetylene from coal, using a plasma jet. Nature, 1963, 200(4913): 1313-1314.
[3] Nicholson R, Littlewood K. Plasma pyrolysis of coal. Nature, 1972, 236(5347): 397-400.
[4]许根慧,姜恩永,盛京.等离子体技术与应用.北京:化学工业出版社, 2006.
[5]过增元,赵文华.电弧和热等离子体.北京:科学出版社, 1986. pp3-4.
[6] Boulos M I, Fauchais P, Pfender E. Thermal plasmas: fundamentals and applications (Vol. 1). New York: Plenum Press, 1994.
[7]数据来源: Encyclopedia Britannica Online.
[8] Fu Y C, Blaustei B D. Reactions of coal and related materials in microwave discharges in hydrogen water vapour and argon. Fuel, 1968, 47: 463.
[9] Djebabra D. Coal-gasification by microwave plasma in water-vapor. Fuel, 1991, 70: 1473-1475.
[10] Bystrzejewski M, Huczko A, Lange H, Potczyk W W, Stankiewicz R, Pichler T, Gemming T, Rümmeli M H. A continuous synthesis of carbon nanotubes by DC thermal plasma jet. Applied Physics A, 2008, 91: 223-228.
[11] Georgiev I B, Mihailov B I. Some general conclusion from the results of studies on solid fuel steam plasma gasification. Fuel, 1992, 71: 895-901.
[12] Kawamura K, Hirasawa A. Pilot plant experiment of NOx and SO2 removal from exhaust gases by electronbeam irradiation. Radiate. Phys. Chem. 1979, 13: 5-12.
[13] Tokunaga O, Suzuki N. Radiation chemical reactions in NOx and SO2 removals from flue gas. Radiate. Phys. Chem. , 1990, 24: 145-165.
[14]邰德荣,韩宾兵.电子束烟气脱硫示范工程.华东电力, 1999, 3: 5-8.
[15] Ohkubo T, Kanazawa S, Nomoto Y, Chang J, Adachi T. NOx removal by a pipe with nozzle - plate electrode corona discharge system. IEEE trans. on Indus. App., 1994, 30: 856-860.
[16] Chang J S. Lawless P A, Yamamoto T. Corona discharge processes. IEEE Trans. on Plasma Science, 1991, 19: 1152-1165.
[17]顾璠,叶丹.低温等离子体吸附催化烟气脱硫装置及其脱硫方法:中国: 1597057[P], 2005-03-23.
[18]顾璠,余刚,徐益谦.表面吸附低能态等离子体一氧化氮脱除方法.中国专利, 1486775, 2004-04-07.
[19] Huang, A. M., Xia, G. G.,Wang, J. Y., et al. CO2 reforming of CH4 by atmospheric pressure as discharge plasmas. Journal of Catalysis, 2000, 189: 349-359.
[20] Jiang T, Zhang K, Liu C J. Co-generation of syngas and hydrocarbons from methane and carbon dioxide using dielectric barrier discharges. Journal of Fuel Chemistry and Technology, 2001, 29: 6-11.
[21] Wang Q, Yan B H, Jin Y, Cheng Y. Investigation of Dry Reforming of Methane in a Dielectric Barrier Discharge Reactor. Plasma chemistry and plasma processing. 2009, 29: 217-228.
[22] Wang Q, Yan B H, Jin Y,Cheng Y. Dry Reforming of Methane in a Dielectric Barrier Discharge Reactor with Ni/Al2O3 Catalyst: Interaction of Catalyst and Plasma. Energy and fuels, 2009, 23: 4196-4201.
[23] Wang Q, Cheng Y, Jin Y. Dry reforming of methane in an atmospheric pressure plasma fluidized bed with Ni/γ-Al2O3 catalyst . Catalysis today, 2009, 148: 275-282.
[24] Yan B H, Wang Q, Jin Y, Cheng Y. Dry Reforming of Methane with Carbon Dioxide Using Pulsed DC Arc Plasma at Atmospheric Pressure. Plasma chemistry and plasma processing, 2010, 30: 257-266.
[25] Wu C N, Chen J Q, Cheng Y. Thermodynamic analysis of coal pyroysis to acetylene in hydrogen plasma reactor. Fuel processing technology, Fuel Process. Technol., 2009, doi: 10.1016/j.fuproc.2009.09.013.v
[26] Fauchais P, Bourdin E, Aubreton J, Amouroux J. Plasma chemistry and its applications to the synthesis of acetylene from hydrocarbons and coal. International Chemical Engineering, 1980, 20(2): 289-305.
[27] Chakravartty S C, Dutta D, Lahiri A. Reaction of coals under plasma conditions: direct production of acetylene from coal. Fuel, 1976, 55, 43–46.
[28] Chakravartty S C, Dixit L P, Srivastava S K. Hydrogen enriched plasma for direct production of acetylene from coal. Indian Journal of Technology, 1984, 22: 146-150.
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[79]数据来源:http://baike.baidu.com/view/968292.htm
[80]数据来源:http://www.safe.gov.cn/model_safe/tjsj/rmb_list.jsp?ct_name=人民币汇率中间价&id=5&ID=110200000000000000
[81]数据来源:http://www.chemcp.com/news/price/meitan/.