鼓泡淤浆床甲醇合成(Ⅱ)工业装置的工程分析

利用经热模试验验证的鼓泡淤浆床甲醇合成的数学模型 ,讨论了不同参数 ,如表观气速、反应器直径、床层高度等对床层颗粒轴向分布的影响规律 ,确定了万吨级三相床甲醇合成工业示范装置的主要结构参数和操作参数范围 .对两种不同工业原料气分别进行了模拟计算 .模拟结果表明 ,在三相床甲醇合成过程中 ,压力的影响最为显著 ,反应器内床层高度亦是较为重要的可调节参数 .在本文的操作条件下 ,当甲醇产量达到 1× 10 4t·a^-1时 ,在较广的温度和压力范围内 ,对两种原料气 ,出口甲醇摩尔分数在 7%～ 10 % ,CO转化率为 40 %～5 0 %     

乙烯氧化固定床反应器温度场模拟研究

针对乙烯氧化制环氧乙烷固定床反应器,利用YS-7型银催化剂的宏观反应动力学模型和固定床反应器拟均相二维数学模型方法,建立了催化剂床层的质量、热量平衡方程组,并采用Crank-Nicholson差分法对该偏微分方程组进行了数值计算。在模拟计算中,通过改变反应器汽包温度、反应器入口原料气温度、空速以及反应器入口原料气中乙烯、氧气、1,2-二氯乙烷的摩尔分数等工艺条件,系统地研究了以上各工艺条件单因素变化时对整个银催化剂床层温度场的影响。结果表明:随着固定床反应器汽包温度、入口原料气中乙烯、氧气摩尔分数的升高,以及固定床反应器中空速、入口原料气的温度及1,2-二氯乙烷摩尔分数的降低,银催化剂床层温度均有所升高,特别是床层"热点"区域的温度升高较明显。     

大颗粒三相环隙气升式环流反应器流体力学行为

研究了大颗粒体系气升式环流反应器的流体力学行为,考察了表观气速和颗粒质量分数对床层膨胀高度、循环液速和固含率分布的影响。实验结果表明,按颗粒的运动状态不同可以将反应器内的流动分为3个区域,即固定床区域、膨胀床区域和循环床区域,各流动区域内的流动行为存在显著差异。随着颗粒质量浓度的增大,起始流化气速和最小循环气速均显著增大。基于三相流化床的流化模型和环流反应器的特点建立了相应的数学模型,对大颗粒三相气升式环流反应器的起始流化气速和最小循环气速进行了预测,模型预测值与实验测量值吻合良好。     

三相携带床的流体力学特性研究

研究了空气一水-黄沙三相系统在携带床反应器中的流体力学特性。反应器直径0．07m。实验考察了表观气速Ug、表观浆液流速UsL、固含率εs等因素对气含率εg和床层压降△P的影响以及三相携带床的操作特性。回归实验数据得到气含率及床层压降与各因素的关联式为εg=0.4084U△P=5783．672U研究结果为三相携带床工业反应器提供了流体力学依据。     

三相淤浆床甲醇含成反应器大型冷模研究

以空气-水-催化剂和空气-液体石蜡油-催化剂两种系统为对象,研究了内置垂直管束式换热器三相淤浆床甲醇合成反应器的流体力学性质──平均气含率、床层压降、固体完全悬浮的临界表观气速。考察了各种因素对流体力学性质的影响,并得到关于气含率的经验关联式：     

浆态床鼓泡反应器中气含率的分布

为了解浆态床鼓泡反应器中气含率的分布规律,在浆态床鼓泡反应器冷模试验装置中,以空气-液体石蜡-氧化铝微球为试验介质对装置内部的气含率进行研究。利用压差法研究了表观气速、浆液固含量等操作条件对反应器床层总体气含率的影响,利用光纤探针法研究了浆态床反应器不同操作条件对局部气含率的影响,总结了反应器内部气含率的分布规律,并由此对工业浆态床鼓泡反应器的设计进行了研究。结果表明:浆态床反应器的总体气含率随表观气速的增大而增大,固体细颗粒的加入能适当降低总体气含率;在反应器底部,分布器对气体的均布作用明显,但表观气速的增大能够弱化分布器的作用;在反应器的中上部气含率不受分布器的影响,沿反应器径向呈现"中间高,边缘低"的分布趋势;在工业费托浆态床中,表观气速不宜低于0.12 m/s,内过滤系统适宜设置于反应器中上部靠近器壁的位置。     

三相滴流床反应器基于CFD的模拟方法探究

滴流床反应器是一种典型的气液固三相反应器,广泛应用于化学与石油加工工程。相间、相内传质以及催化剂表面相互作用、催化剂的有效润湿率、反应器流体力学、反应器模型等这些因素都影响着滴流床的反应性能。文章采用的滴流床反应器即是在固体催化颗粒床层内气液两相反应物自上而下流动(沿重力方向)的一类反应器。苯二酚是重要的精细化工中间体,用途非常广泛。我们采用CFD模拟了苯酚氧化生成苯二酚的反应。用网格划分粗细的影响及床层催化剂空隙率对流场的影响,计算为三维模拟计算。模拟了局部气含率、持液量,压力降,轴向速度分布及其径向分布速度等数据,探究了模拟方法,为进一步研究提供了参考依据。     

微膨胀床渣油加氢处理反应器的研究

为考察微膨胀床渣油加氢处理反应器的气液流动状态、床层膨胀率及反应性能,常温、常压下用模拟油气在冷模实验装置上进行了近似模拟,并采用微膨胀床/固定床中型实验装置处理了中东高硫渣油。结果表明:按返混程度微膨胀床反应器可分为3个区域;大粒径、低堆密度催化剂易膨胀;空塔气速对床层膨胀率影响大于空塔液速;中型实验装置可脱除渣油中80%以上硫和钒以及50%以上镍和残炭,其中微膨胀床脱除率占50%以上。     

上流式反应器气液相间传质特性的实验研究

上流式反应器设置在固定床渣油加氢反应器前有利于提高渣油原料适用性,延长装置运行时间。实验研究了上流式反应器气液相间传质,采用五齿柱形氧化铝催化剂模拟工业催化剂颗粒,水溶液模拟渣油,空气模拟氢气,采用无氧水物理吸收和亚硫酸钠化学吸收的方法,测定了在高气液比的条件下上流式反应器床层气液相间传质特性实验。考察了表观气速、表观液速、填料粒径、内构件、催化剂级配和床层高径比对液相体积传质系数和气液相界比表面积的影响规律。实验数据表明,液相体积传质系数随着气、液速的增大而增大;随填料颗粒增大而减小;在床层内安装合适的内构件或增大反应器高径比,能够促进气液相间传质。基于实验数据拟合了适合上流式反应器液相体积传质系数和气液相界比表面积的经验关联式,拟合误差最大分别为12%和24%;表明所建气液相间传质的经验关联式能更好地预测上流式反应器中的气液相间传质特性。     

上流式反应器气液相间传质特性的实验研究

上流式反应器设置在固定床渣油加氢反应器前有利于提高渣油原料适用性,延长装置运行时间。实验研究了上流式反应器气液相间传质,采用五齿柱形氧化铝催化剂模拟工业催化剂颗粒,水溶液模拟渣油,空气模拟氢气,采用无氧水物理吸收和亚硫酸钠化学吸收的方法,测定了在高气液比的条件下上流式反应器床层气液相间传质特性实验。考察了表观气速、表观液速、填料粒径、内构件、催化剂级配和床层高径比对液相体积传质系数和气液相界比表面积的影响规律。实验数据表明,液相体积传质系数随着气、液速的增大而增大;随填料颗粒增大而减小;在床层内安装合适的内构件或增大反应器高径比,能够促进气液相间传质。基于实验数据拟合了适合上流式反应器液相体积传质系数和气液相界比表面积的经验关联式,拟合误差最大分别为12%和24%;表明所建气液相间传质的经验关联式能更好地预测上流式反应器中的气液相间传质特性。     

Hydrodynamics of an annulus airlift reactor

The hydrodynamics of an annulus airlift reactor (AALR) was studied and compared with that of a slurry bubble column reactor (SBCR) with silica sands of 75-125 μm in size as solids, city tapping water as liquid phase, and air as gas phase in the present investigation. The effects of superficial gas velocity and solids concentration on gas holdup and solids distributions were investigated. The results showed that the local average gas holdup decreased along the column height, and the average gas holdup decreased with the increasing solids concentration, but this tendency became less at higher solids concentrations. It was found that the effect of superficial gas velocity on axial solids distribution was negligible over the gas velocity range investigated, as long as the solids in the column could be suspended. Increasing solids concentration led to flatter axial solids holdup profiles. The axial distributions of solids concentration and gas holdup in the AALR were much more uniform than those in the SBCR, and slurry circulation in the AALR damped the effects of increasing solids concentration on the hydrodynamics. These advantages of an AALR over a SBCR are especially important for some catalytic reaction processes in three-phase systems such as Fischer-Tropsch synthesis and methanol synthesis.     

鼓泡淤浆床甲醇合成(Ⅰ)数学模型及试验验证

建立了一套Φ0 .2m鼓泡淤浆反应器热模试验装置 ,并完成了连续运行 10 0 0h的装置可操作性与稳定性考核试验 .试验中 ,合成反应温度 498～ 5 2 5K ,压力 2 .5～ 3 .1MPa ,质量空速 45 0 0～ 75 0 0L·kg^-1·h^-1,原料气中CO摩尔分率 0 .31.结合热模试验及合成系统的特点 ,得到了计入液相轴向返混、催化剂颗粒轴向分布及气 -固相本征动力学的数学模型 .由该模型得到的甲醇产率及出口甲醇摩尔分率的计算值与热模试验值吻合良好 .将合成压力外推至 5 .0MPa ,通过验证后的模型所得到的模拟数据与美国中试结果相当 ,表明热模试验中所采用的国产C30 2催化剂与医用液体石蜡惰性溶剂互适性良好     

Multicompartment hydrodynamic model for slurry bubble columns

A core-annulus multicompartment two-dimensional two-bubble class model accounting for slurry recirculation and coupled with catalyst transport was developed as a part and parcel of the analysis of the behavior of slurry bubble column reactors at high gas throughputs corresponding to the churn turbulent flow regime. The model analyzed the contributions of bubble-induced turbulence closures, bubble coalescence and breakup phenomena, and catalyst axial distribution as the resultant of sedimentation, advection via liquid-solid slip, per-compartment axial dispersion and core-annulus lateral exchange of catalyst by bubble-induced turbulence. The model was also used to analyze the effects of catalyst loading, gas density and superficial velocity, and column diameter and vessel aspect ratio on the hydrodynamics of slurry bubble column reactors, namely, the per-compartment phase holdups and interstitial velocities, pressure gradient, bubble coalescence and break-up rates, and loci of velocity inversion for the gas and slurry profiles.     

高温高压浆态鼓泡床反应器中的气-液传质

The gas-liquid mass transfer of H2 and CO in a high temperature and high-pressure three-phase slurry bubble column reactor is studied. The gas-liquid volumetric mass transfer coefficients kLa are obtained by measuring the dissolution rate of H2 and CO. The influences of the main operation conditions, such as temperature, pressure,superficial gas velocity and solid concentration, are studied systematically. Two empirical correlations are proposed to predict kLa values for H2 and CO in liquid paraffln/solid particles slurry bubble column reactors.     

A novel slurry bubble column membrane reactor concept for Fischer–Tropsch synthesis in GTL technology

Fischer–Tropsch synthesis (FTS) plays an important role in the production of ultra-clean transportation fuels, chemicals, and other hydrocarbon products. In this work, a novel combination of fixed-bed and slurry bubble column membrane reactor for Fischer–Tropsch synthesis has been proposed. In the first catalyst bed, the synthesis gas is partially converted to hydrocarbons in a water-cooled reactor which is fixed bed. In the second bed which is a membrane assisted slurry bubble column reactor, the heat of reaction is used to preheat the feed synthesis gas to the first reactor. Due to the decrease of H₂/CO to values far from optimum reactants ratio, the membrane concept is suggested to control hydrogen addition. A one-dimensional packed-bed model has been used for modeling of fixed-bed reactor. Also a one-dimensional model with plug flow pattern for gas phase and an axial dispersion pattern for liquid-solid suspension have been developed for modeling of slurry bubble column reactor. Proficiency of a membrane FTS reactor (MR) and a conventional FTS reactor (CR) at identical process conditions has been used as a basis for comparison in terms of temperature, gasoline yield, H₂ and CO conversion as well as selectivity. Results show a favorable temperature profile along the proposed concept, an enhancement in the gasoline yield and, thus a main decrease in undesirable product formation. The results suggest that utilizing this type of reactor could be feasible and beneficial. Experimental proof of concept is needed to establish the validity and safe operation of the proposed reactor.     

费托合成浆态床速度分布和浓度分布的模拟及其影响规律

提出了浆态床速度分布的一维流体力学模型和合成气液相浓度分布的二维扩散模型,用于描述浆态床液相返混对费托合成反应的影响。模型计算结果与示范工厂数据符合良好。计算表明,液相返混状态对合成气转化率有显著影响。利用模型考察了空塔气速对合成气转化率和空时产率的影响规律,随气速增加,合成气转化率单调下降,空时产率先增大后缓慢降低;塔径放大后,中心液速和液相循环流率都增大,浆料返混加剧,费托合成反应转化率降低。     

Modelling-based Optimisation of the Direct Synthesis of Dimethyl Ether from Syngas in a Commercial Slurry Reactor

In the present study, we developed a multi-component one-dimensional mathematical model for simulation and optimisation of a commercial catalytic slurry reactor for the direct synthesis of dimethyl ether (DME) from syngas and CO₂, operating in a churn-turbulent regime. DME productivity and CO conversion were optimised by tuning operating conditions, such as superficial gas velocity, catalyst concentration, catalyst mass over molar gas flow rate (W/F), syngas composition, pressure and temperature. Reactor modelling was accomplished utilising mass balance, global kinetic models and heterogeneous hydrodynamics. In the heterogeneous flow regime, gas was distributed into two bubble phases: small and large. Simulation results were validated using data obtained from a pilot plant. The developed model is also applicable for the design of large-scale slurry reactors.     

浆料鼓泡塔反应器部分流体力学参数研究综述

本文综述了浆料鼓泡塔反应器的主要流体力学参数－流域,气泡的大小和上升速度,相含率和固定颗粒悬浮的临床气速等－的测定和影响因素。简要介绍了国外采用的汉体力学参数测定方法－动态气体逸出法。