摘要
本文以天然气制合成油(GTL)核心技术之一的天然气非催化部分氧化制备合成气转化炉技术的大型化为目标,以天然气非催化转化技术的工业应用实践为基础,研究了转化炉大型化工艺操作条件的优化选择、转化烧嘴与炉体合理匹配等关键技术的理论依据和放大方法,提出了适于百万吨/年GTL合成油装置用大型化天然气非催化部分氧化转化炉系统集成的可实施技术方案。概要如下：
1.通过对已有的天然气非催化部分氧化转化过程研究结果及其关键技术的分析和热力学平衡计算,探讨了转化炉工艺操作条件对转化结果的影响,提出了优化的大型天然气非催化部分氧化转化炉工艺操作条件。
2.采用大型冷模实验和数值模拟相结合的方法,研究了转化炉冷态流场。在(?)1000mm大型冷模实验装置上重点研究了转化炉内的轴向速度和炉内气体停留时间分布,通过冷态流场数值模拟计算,验证了实验研究与数值模拟结果的符合性。
3.采用概率密度函数模型(PDF)模型,研究了现有工业运行装置和未来大型转化炉内流动和反应的状况,考察了工艺条件对大型转化炉内流动与反应过程的影响。模拟结果表明：大型转化炉与已工业运行转化炉两者的炉内流动与混合基本相似；降低氧气入口温度对降低转化炉拱顶附近的温度作用不明显；提高氧气入口温度可以降低拱顶温度；增加水蒸汽量虽然在一定程度上降低拱顶的气体温度,但火焰位置并没有显著的下移。
4.采用稳态传热理论和灵敏度分析方法,从理论上印证了影响转化炉拱顶外壁温度的关键因素为耐火隔热衬里层各物性参数中的莫来石隔热砖导热系数；采用CFD数值模拟方法,建立了多孔隔热材料的微观结构模型、微观传热物理模型和数学模型,进行了微观传热过程的数值模拟,研究了莫来石隔热砖材料表观(实际)导热系数与转化炉内操作温度、含氢气氛及微观结构尺度(粒径大小及开口气孔率)之间的变化规律和量化关系,提出了转化炉内环境45-70%含氢量气氛下多孔隔热材料的表观(实际)导热系数的预测方法,工业运行转化炉的应用验证表明与实测数据具有较好的偏离度(小于6%),可以指导转化炉拱顶隔热衬里层设置的工程设计；建立了转化炉拱顶耐火隔热衬里衬里层传热过程的整体物理模型,进行了全尺寸、变物性多物理场的整体传热模拟。结果表明：大型天然气转化炉拱顶隔热衬里的温度分布特点与工业运行装置转化炉拱顶基本相似,验证了该拱顶隔热衬里层设计的正确性。
5.在总结天然气非催化部分氧化的工业化成功工程实践的基础上,建立了适于百万吨/年规模GTL合成油装置的大型天然气非催化部分氧化工艺集成系统,提出了可实施的大型天然气非催化转化关键设备设计和单系列工艺流程的技术方案。该技术方案表明：大型转化炉生产有效合成气(CO+H2)147,100Nm3/h,大然气转化系列数和转化炉数量为5个系列5台,单台转化炉对应的合成油产量为20万吨/年；烧嘴采用与工业成功运行烧嘴相同的物料流道设置技术,为氧气(少量)-氧气(大量)天然气—保护蒸汽四通道；工艺流程可划分为天然气转化工序、合成气热量回收工序和合成气洗涤工序;工艺系统的物料热量模拟计算结果与工业运行装置的实际操作数据基本相同,冷煤气效率为84%,总能量利用效率为99%。
This paper, by taking the large-scale industrial reformer technology for making syngas (CO+H2) by the process of natural gas non-catalytic partial oxidation (POX) being one of the key technologies for synthetic oil production from natural gas (GTL) as the objective and the practical industrial applications of natural gas non-catalytic conversion technology as the basis, has studied both the theoretical basis and enlargement methods for such key technologies as optimized selection of process operation conditions for large-scale industrial reformer and reasonable match of burner with reformer, and put forward some implemented technical solutions in the integration of large-scale industrial reformer system employing natural gas non-catalytic POX process for setting up a GTL unit in the capacity producing a million tons of synthetic oil. A summary is as follows:
1. With the study results of existing conversion process of natural gas non-catalytic POX and the analysis of its related technologies as well as the thermodynamic equilibrium calculations, the effects on the conversion results by process operation conditions in reformer have been discussed and the principles in optimized selection of process operation conditions in large-scale reformer employing natural gas non-catalytic POX put forward.
2. The cold flow field in reformer has been studied by the two approaches of both large-scale experiment of cold model and numerical simulation. The study focusing on both the axial velocity and the residence time distribution of gas in the reformer have been carried out on a large-scale cold test device of 01000mm;the result compliance of experimental study and numerical simulation have been verified with the simulation calculations of cold flow field.
3. The status of flow and reaction both in the existing industrial operating plant and large-scale reformer have been studied and simulated by taking the selected probability density function (PDF) model and the effect on both the flow and reaction in large-scale reformer by process conditions investigated. The simulation results show that both the flow and mix in large-scale reformer and industrial operating reformer are similar; the effect in reducing the inlet oxygen temperature is not obvious in reducing the temperature in the vicinity of reformer vault whereas increasing inlet oxygen temperature may reduce vault temperature; though increasing the steam amount may reduce the gas temperature on vault to a certain extent, yet the flame position has not shown a significant movement downward.
4. By taking a steady heat-transfer theory and a sensitivity analysis it is theoretically confirmed that the key factor affecting the outer-wall temperature of reformer vault is being the thermal conductivity of Mullite insulation bricks in the various physical parameters of refractory insulation lining; a micro-structural model of porous insulation material, a micro-physical model of heat transfer and a mathematical model have been set up by taking a CFD numerical simulation for numerical simulation of micro process of heat transfer in the study of variation laws and quantitative relationship between the apparent (actual) thermal conductivity of Mullite insulation bricks and the operating temperature, hydrogen atmosphere and micro-structural scale (particle size and open porosity), and a prediction method for a apparent (actual) thermal conductivity of porous insulation material at 45-70% hydrogen atmosphere inside reformer has been proposed; the application verification of industrial operating reformer shows a better deviation (less than 6%) which may guide the arrangement engineering design of insulation lining on reformer vault; an integral physical model of heat transfer process on refractory insulation lining of reformer vault has been established and an integral simulation of heat transfer in full size with variable physical properties and multi-physical fields has been carried out. The results show that the temperature distribution features of insulation lining on large-scale natural gas reformer vault are similar to that of industrial operating plant, thus, the correctness in the design of this vault insulation lining has been verified.
5. Based upon a summary of engineering practice of successful industrialization of natural gas non-catalytic POX, a large-scale process integration system of natural gas non-catalytic POX for a GTL plant in a million-ton capacity has been set up, an implemented technical scheme for the design of critical equipment and a process flows of a single train of large-scale natural gas non-catalytic conversion technology proposed. The said scheme shows that (1) a large-scale reformer produces an effective syngas (CO+H2) 147,100Nm3/h with 5 trains of natural gas conversion and 5 reformers, the yield of synthetic oil from each single reformer is 200,000t/a; (2) burner uses the same design technique for the arrangement of stream flows as that in the successful industrial operation being 4 channels of oxygen (small amount)-oxygen (large amount)-natural gas-protective steam; (3) process flows may be divided into sections of natural gas conversion, syngas heat recovery and syngas scrubbing; (4) the simulated heat calculation results of process system are basically the same as the actual operating data from industrial operating plant, the efficiency of cold gas is 84% and the total energy efficiency,99%.
引文
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