煤直接液化强制循环淤浆床反应器工程化研究
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摘要
我国煤炭资源丰富,煤炭直接液化技术不仅能提高煤炭资源的利用效率,弥补国内石油的空缺,而且可以减少煤炭直接燃烧对环境造成的污染,是解决当前我国能源短缺和石油安全的重要途径之一,具有重要的战略意义、现实意义和经济价值。为配合我国神华大型煤直接液化工业生产装置的建设,对神华煤直接液化反应器现有工程化实践进行理论分析和总结,且在应用基础方面开展深入研究,可为这类反应器的工程设计和放大、过程优化和控制提供理论基础和技术支持。鉴此,本文采用工程试验和模型化方法,针对神华煤直接液化反应工艺中强制循环淤浆床反应器的多相流动和反应性能,较为系统地开展了该类反应器的工程化应用基础研究。
首先,通过对神华煤直接液化反应工艺及反应器技术的论证分析表明,采用浆相强制循环操作模式的淤浆床反应器在控制反应器内温度均匀,实现固体颗粒充分流化,以及减小器内气体滞留、提高反应器空间利用率等方面均具有优势。
其次,在实验室尺度,分别以空气和水为气、液相,以玻璃珠和煤粉为固相,在φ200×2500mm的冷模反应器中实验测定了强制循环淤浆床反应器的流动性能,系统考察了反应器结构、操作条件及物性对器内流动性能的影响,揭示模拟重颗粒流化的“玻璃珠-水-空气”三相体系、模拟煤液化的“煤-水-空气”三相体系中的压强分布和脉动、相分散(床层整体气、固含率及局部分布)和浆相环流特性。而且,针对原料煤钙含量高、液化时易聚集问题的模拟侧壁放料试验表明,反应器中累积的密度较大的玻璃珠,可以通过侧壁放料有效排除。
第三,在中试尺度(6吨干煤／天规模)的PDU装置上,开展了热态、真实反应条件下煤直接液化强制循环反应器的流动及反应性能的工程化试验,结果表明：1)PDU装置可用于热态反应条件下的反应器流动性能测试,连续运行过程中各项参数都达到了预期值；2)通过对PDU装置液化反应器底部气含率的测定,得出热模状态下第一液化反应器底部气含率关联式为：3)非反应状态下,内循环反应器和强制循环反应器内的返混强度远远大于鼓泡床反应器；非反应状态和煤直接液化反应状态下,内循环反应器和强制循环反应器有着相近的循环强度和返混强度；4)在操作条件接近的情况下,强制循环反应器和内循环反应器有着非常接近的原料煤转化率；其中,在试验操作条件下使用强制循环反应器可避免钙粒子的沉积现象。
第四,应用商用计算流体力学(CFD)软件FLUENT,对PDU装置强制循环反应器的流动性能进行了CFD模拟,分析计算所得反应器模拟区域的气含率、湍动能、压力以及液相速度的分布,揭示了器内流动参数的局部分布特征；其中,预测整个区域气含率等,与冷模试验结果相近。
最后,在基于对PDU装置煤液化反应器性能的基本假设上,建立了一个简单的神华煤直接液化强制循环反应器模型。计算初步表明,对于神华煤的两段反应器过程,长的平均停留时间,大的反应速率常数,均有助于提高对应组分的转化或生成；较之日本NEDOL工艺及所用煤种(印尼Tanitoharum煤),神华工艺及所用神华煤似有短停留时间、高转化率的特点。
Coal is the most abundant fossil fuel in China. Hence, it is strategically and economically important to develop coal liquefaction technologies as an effective way to solve the oil and energy shortage problem in our country, and in the meanwhile to avoid environmental pollution and wastes and utilize coal cleanly and effectively. Towards the end, a commercial plant of large scale production capacity has been constructed by Shenhua for producing the direct coal liquefaction oil. For the successful process design, scale up and its optimization and control, it is inevitable to derive process and engineering knowledge from the successful practice of the Shenhua direct coal liquefaction process, and implement further fundamental studies on the process. In this paper, a systematic engineering research was carried with a particular focus on the multiphase flow and reaction performances of forced recirculating slurry bed reactor used for the Shenhua coal liquefaction process.
In the first place, a detailed analysis of the Shenhua direct coal liquefaction process and the reactor technology shows that a slurry bed reactor operated in the forced circulating mode of the slurry phase presents advantages such as uniform temperature distribution, good fluidization of large and heavy solid particles, and less degree of gas retention and thus effective utilization of reactor space, all of which are necessary for the highly exothermal coal liquefaction process.
Secondly, on the lab scale, three phase flow hydrodynamics in a cold model slurry bed reactor of 2500 mm high and 200mm in diameter were experimentally studied, using air as the gas phase, water as the liquid phase, and glass beads or coal powders as the solid phase. The pressure distribution and its fluctuation, phase dispersion (overall and local gas and solid hold-ups) and liquid circulation velocity were measured in two systems, namely, the coal/water/air system that mimics the coal liquefaction suspensions, and the glass bead/water/air system that approximates the situation where deposition of minerals may occur during coal liquefaction; and the influence of reactor configuration, operation condition, and phase properties on the three phase flow hydrodynamics was systematically investigated. Besides, in view of the high content of calcium in Shenhua coal and tendency to solid deposition in liquefaction, simulating discharge experiments of high density glass beads via the reactor side wall were carried out and shown to be an effective method of solving the deposition problem in the liquefaction process.
Thirdly, on the pilot plant scale, flow and reaction performances of a hot model forced circulation slurry bed reactor in a process supporting unit (PDU) with a capacity of 6 ton dry coal/day were investigated, and a collection and analysis of the process data was made. It is demonstrated that 1) the PDU system were successfully operated with process parameters attaining the desired ones, and properly designed for evaluating the flow and reaction performances of the PDU reactor; 2) the gas hold-up at the bottom of the PDU reactor was measured and determined by the following correlation 3) a comparison of slurry circulation intensity between three different liquefaction multiphase reactors, i.e., the PDU reactor of forced circulation of the slurry phase, a internal circulation reactor with a draft tube, and the conventional slurry bed reactor without internals, shows that the former two reactors are identical to each other and superior to the conventional one in terms of their circulation intensity; and 4) the former two reactors exhibit approximately the same coal conversions, and the PDU reactors were found to be nearly free of the calcium deposition problem owing to the intensive and forced slurry circulation.
Fourthly, hydrodynamic performances of the PDU reactor were simulated by using the computational fluid dynamics (CFD) method and the FLUENT software. Spatial distribution of flow parameters, including the gas hold-up, turbulent kinetic energy, pressure and liquid velocity, was obtain and thereby used to ascertain the local distribution characteristics of flow parameter within the reactor. Predicted gas hold-up values are found to be close to those measured in the cold model reactor.
Lastly, with basic assumptions, a simple reactor simulation model was developed for predicting the reaction performance of the two coal direct liquefaction reactors in the PDU process. It is shown that for the liquefaction of the Shenhua coal in the two reactors, longer mean residence time/higher reaction coefficients are favorable for the transformation or formation of corresponding product species; and compared to the NEDOL process and the Tanitoharumis used therein, the Shenhua process and the coal used exhibit characteristic of shorter residence time but higher conversions.
首先,通过对神华煤直接液化反应工艺及反应器技术的论证分析表明,采用浆相强制循环操作模式的淤浆床反应器在控制反应器内温度均匀,实现固体颗粒充分流化,以及减小器内气体滞留、提高反应器空间利用率等方面均具有优势。
其次,在实验室尺度,分别以空气和水为气、液相,以玻璃珠和煤粉为固相,在φ200×2500mm的冷模反应器中实验测定了强制循环淤浆床反应器的流动性能,系统考察了反应器结构、操作条件及物性对器内流动性能的影响,揭示模拟重颗粒流化的“玻璃珠-水-空气”三相体系、模拟煤液化的“煤-水-空气”三相体系中的压强分布和脉动、相分散(床层整体气、固含率及局部分布)和浆相环流特性。而且,针对原料煤钙含量高、液化时易聚集问题的模拟侧壁放料试验表明,反应器中累积的密度较大的玻璃珠,可以通过侧壁放料有效排除。
第三,在中试尺度(6吨干煤／天规模)的PDU装置上,开展了热态、真实反应条件下煤直接液化强制循环反应器的流动及反应性能的工程化试验,结果表明：1)PDU装置可用于热态反应条件下的反应器流动性能测试,连续运行过程中各项参数都达到了预期值；2)通过对PDU装置液化反应器底部气含率的测定,得出热模状态下第一液化反应器底部气含率关联式为：3)非反应状态下,内循环反应器和强制循环反应器内的返混强度远远大于鼓泡床反应器；非反应状态和煤直接液化反应状态下,内循环反应器和强制循环反应器有着相近的循环强度和返混强度；4)在操作条件接近的情况下,强制循环反应器和内循环反应器有着非常接近的原料煤转化率；其中,在试验操作条件下使用强制循环反应器可避免钙粒子的沉积现象。
第四,应用商用计算流体力学(CFD)软件FLUENT,对PDU装置强制循环反应器的流动性能进行了CFD模拟,分析计算所得反应器模拟区域的气含率、湍动能、压力以及液相速度的分布,揭示了器内流动参数的局部分布特征；其中,预测整个区域气含率等,与冷模试验结果相近。
最后,在基于对PDU装置煤液化反应器性能的基本假设上,建立了一个简单的神华煤直接液化强制循环反应器模型。计算初步表明,对于神华煤的两段反应器过程,长的平均停留时间,大的反应速率常数,均有助于提高对应组分的转化或生成；较之日本NEDOL工艺及所用煤种(印尼Tanitoharum煤),神华工艺及所用神华煤似有短停留时间、高转化率的特点。
Coal is the most abundant fossil fuel in China. Hence, it is strategically and economically important to develop coal liquefaction technologies as an effective way to solve the oil and energy shortage problem in our country, and in the meanwhile to avoid environmental pollution and wastes and utilize coal cleanly and effectively. Towards the end, a commercial plant of large scale production capacity has been constructed by Shenhua for producing the direct coal liquefaction oil. For the successful process design, scale up and its optimization and control, it is inevitable to derive process and engineering knowledge from the successful practice of the Shenhua direct coal liquefaction process, and implement further fundamental studies on the process. In this paper, a systematic engineering research was carried with a particular focus on the multiphase flow and reaction performances of forced recirculating slurry bed reactor used for the Shenhua coal liquefaction process.
In the first place, a detailed analysis of the Shenhua direct coal liquefaction process and the reactor technology shows that a slurry bed reactor operated in the forced circulating mode of the slurry phase presents advantages such as uniform temperature distribution, good fluidization of large and heavy solid particles, and less degree of gas retention and thus effective utilization of reactor space, all of which are necessary for the highly exothermal coal liquefaction process.
Secondly, on the lab scale, three phase flow hydrodynamics in a cold model slurry bed reactor of 2500 mm high and 200mm in diameter were experimentally studied, using air as the gas phase, water as the liquid phase, and glass beads or coal powders as the solid phase. The pressure distribution and its fluctuation, phase dispersion (overall and local gas and solid hold-ups) and liquid circulation velocity were measured in two systems, namely, the coal/water/air system that mimics the coal liquefaction suspensions, and the glass bead/water/air system that approximates the situation where deposition of minerals may occur during coal liquefaction; and the influence of reactor configuration, operation condition, and phase properties on the three phase flow hydrodynamics was systematically investigated. Besides, in view of the high content of calcium in Shenhua coal and tendency to solid deposition in liquefaction, simulating discharge experiments of high density glass beads via the reactor side wall were carried out and shown to be an effective method of solving the deposition problem in the liquefaction process.
Thirdly, on the pilot plant scale, flow and reaction performances of a hot model forced circulation slurry bed reactor in a process supporting unit (PDU) with a capacity of 6 ton dry coal/day were investigated, and a collection and analysis of the process data was made. It is demonstrated that 1) the PDU system were successfully operated with process parameters attaining the desired ones, and properly designed for evaluating the flow and reaction performances of the PDU reactor; 2) the gas hold-up at the bottom of the PDU reactor was measured and determined by the following correlation 3) a comparison of slurry circulation intensity between three different liquefaction multiphase reactors, i.e., the PDU reactor of forced circulation of the slurry phase, a internal circulation reactor with a draft tube, and the conventional slurry bed reactor without internals, shows that the former two reactors are identical to each other and superior to the conventional one in terms of their circulation intensity; and 4) the former two reactors exhibit approximately the same coal conversions, and the PDU reactors were found to be nearly free of the calcium deposition problem owing to the intensive and forced slurry circulation.
Fourthly, hydrodynamic performances of the PDU reactor were simulated by using the computational fluid dynamics (CFD) method and the FLUENT software. Spatial distribution of flow parameters, including the gas hold-up, turbulent kinetic energy, pressure and liquid velocity, was obtain and thereby used to ascertain the local distribution characteristics of flow parameter within the reactor. Predicted gas hold-up values are found to be close to those measured in the cold model reactor.
Lastly, with basic assumptions, a simple reactor simulation model was developed for predicting the reaction performance of the two coal direct liquefaction reactors in the PDU process. It is shown that for the liquefaction of the Shenhua coal in the two reactors, longer mean residence time/higher reaction coefficients are favorable for the transformation or formation of corresponding product species; and compared to the NEDOL process and the Tanitoharumis used therein, the Shenhua process and the coal used exhibit characteristic of shorter residence time but higher conversions.
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