下行床气固传质及反应特性的实验研究

以臭氧催化分解为模型反应,对气固并流下行循环流化床反应器中气固传质与反应特性进行了研究. 制备了臭氧分解催化剂,并以它为循环物料在内径0.09 m、高度8.2 m的下行床中测定了颗粒浓度分布和臭氧浓度分布. 实验结果表明,臭氧在加速段分解率在45%左右,约占总分解率的90%,其随颗粒循环量(Gs)的增加略有上升. 当Gs从2.77 kg/(m2×s)增加到6.58 kg/(m2×s)时,全床分解率从50%上升至55%. 建立了平推流的传质模型,给出了有效传质系数和操作参数的关联式.     

Hydrodynamics and reactor performance evaluation of a high flux gas‐solids circulating fluidized bed downer: Experimental study

Reactor performance of a high flux circulating fluidized bed (CFB) downer is studied under superficial gas velocities of 3–7 m/s with solids circulation rate up to 300 kg/m²s using ozone decomposition reaction. Results show that the reactant conversion in the downer is closely related to the hydrodynamics, with solids holdup being the most influential parameter on ozone decomposition. High degree of conversion is achieved at the downer entrance region due to strong gas‐solids interaction as well as higher solids holdup and reactant concentration. Ozone conversion increases with the increase of solids circulation rate and/or the decrease of superficial gas velocity. Overall conversion in the CFB downer is less than but very close to that in an ideal plug flow reactor indicating a good reactor performance in the downer because of the nearly “ideal” hydrodynamics in downer reactors. © 2014 American Institute of Chemical Engineers AIChE J, 60: 3412–3423, 2014     

Evaluation of downer reactor performance by catalytic ozone decomposition

Radial distribution profiles of ozone concentrations were measured along an 8.50 m high and 0.09 m inside diameter gas/solid co-current down-flow circulating fluidized bed (downer) to characterize the reactor performance. Tests were conducted under a series of operating conditions at room temperature and near atmospheric pressure, with FCC particles as the bed material. Results show that the concentration distribution of the ozone tracer gas correlates well with the flow structure of the downer. There is quite a uniform radial distribution of ozone concentrations in the core region of all tested axial sections in the fully developed region of the downer, except for the near-wall region where there is a sharp decrease in ozone concentration. And there exists a relatively significant non-uniform distribution in the entrance acceleration region of the downer.     

Catalytic reaction in a circulating fluidized bed downer: Ozone decomposition

Catalytic ozone decomposition reaction was used to study the performance of a 76 mm i.d. and 5.8 m high gas–solid circulating fluidized bed (CFB) downer reactor. Optical fiber probes and an ultraviolet (UV) ozone analyzer were used to obtain comprehensive information about local solids holdup and ozone concentration profiles at different axial and radial positions at superficial gas velocity of 2–5 m/s and solids circulation rates of 50 and 100 kg/m² s. Axial ozone concentration profiles significantly deviated from the plug-flow behavior, with most conversion occurring in the entrance region or flow developing zone of the downer reactor. Strong correlation was observed between the spatial distributions of solids and extent of reaction; higher local solids holdups cause lower ozone concentrations due to higher reaction rates. Radial gradients of the reactant (ozone) concentrations increased in the middle section of the downer, and decreased with increasing superficial gas velocity and solids circulation rate. Contact efficiency, a measure of the interaction between gas and solids indicated high efficiency in the flow developing zone and decreased with height in the fully developed region.     

A Comparison of Flow Dynamics and Flow Structure in a Riser and a Downer

Flow development and flow dynamics were systematically investigated using local solids concentration measurements in a pair consisting of a downer (0.1 m I.D., 9.3 m high) and a riser of the same diameter (0.1 m I.D., 15.1 m high). Both statistical and chaos analysis were employed. Values for the Kolmogorov entropy (K), correlation dimension (D), and Hurst exponent (H) were estimated from time series of solids concentration measurements. Axial distributions of chaos parameters were more complex in the downer than those in the riser, especially in the entrance section. Flow in the downer was more uniform with a flatter core in all the radial profiles of chaos parameters. The radial profiles of K varied significantly with increasing axial levels due to different clustering behavior in the wall region of the downer. In both the riser and the downer, anti‐persistent flow in the core region and persistent flow behavior near the wall were identified from the profiles of H. Different flow behavior in the region close to the wall in the downer and riser was characterized from the combination of the three chaos parameters. Relationships between chaos parameters and local time‐averaged solids holdup in the core and wall regions of the developed sections in both the downer and riser were also analyzed.     

Heat Transfer in the Downer and the Riser of a Circulating Fluidized Bed – A Comparative Study

The characteristics of heat transfer were studied in both a gas‐solids concurrent downflow fluidized bed (downer) and a gas‐solids concurrent upflow fluidized bed (riser) with FCC particles. The radial and axial distribution profiles of the heat transfer coefficient between a suspended surface and the gas‐solids flow suspension were obtained using a miniature heat transfer probe, under different operating conditions. Comprising the results of the heat transfer in the downer and the riser shows that there exists some significant distinction between the heat transfer processes in the two reactors. The characteristics of heat transfer in both cases are closely related to their hydrodynamics and the distinct flow structures determinate the different heat transfer behaviors. The results also indicate that the operating conditions present some different effects in the two beds.     

Computer Simulation of the Performance of a Downer‐Regenerator CFB for the Partial Oxidation of n‐Butane to Maleic Anhydride

A reactor model for a downer‐regenerator circulating fluidized‐bed (CFB) during the partial oxidation of n‐butane to maleic anhydride is presented. Upflow reactors (risers) suffer from severe solids back mixing and gas‐solids‐separation, in comparison down flow reactors exhibit a more uniform gas‐solids flow and reduced backmixing, resulting in narrower residence time distributions. Due to the sensitivity of the VPO catalyst to over‐reduction, downer reactors present an interesting alternative to riser reactors. The reactor models for the downer and the regenerator fluidized‐bed are coupled with reduction and oxidation kinetics for the catalyst, respectively. The influence of the solids residence time distributions for the combined system of both reactors on the oxidation state of the catalyst is explored by a novel newly developed oxygen loading distribution. Simulation results suggest the limited solids‐flux in downers restrict the maximum butane concentrations, while the scale‐up is predicted to be uncritical.     

A Comparison of Solids Fluxes in a Pair of Downer and Riser Reactors

A direct comparison on solids flux was enabled by measurements obtained in a pair of riser and downer circulating fluidized bed reactors, of the same diameter, using suction probes. The operating conditions and the axial position were found to affect the solids flux in each reactor in a different manner. The solids flux in the riser were affected to a large degree by the gas velocity, in contrast with the downer where no visible effect was detected from changes in the gas velocity. The axial position has an effect on the shape of the solids flux profiles in the downer, but only small effects were observed in the riser. On the other hand, increases in overall solids flux leads to the increase of local solids flux in both the downer and the riser.     

大型下行式循环流化床反应器颗粒浓度分布研究

采用双光路光纤密度探头研究了内径418mm,高18米大型下行式循环流化床（其中下行床部分长度6．5m)反应器中的颗粒浓度分布，结果表明大直径下行床中颗粒浓度沿径向呈现中心均匀，近壁处存在高浓环形区的分布，这类似于小直径反应器中的结果，随着反应器直径的增加，颗粒浓度分布最大值的径向位置向边壁方向移动，即：当下行床放大时，中心颗粒浓度均匀分布区的面积占整个床层截面积的比例增大，在一种特殊设计的下行床边壁结构中测量了颗粒浓度沿径向的分布，实验结果说明边壁效应对下行床近壁区颗粒浓环的形成起到了重要作用，研究结果将有助于了解下行床反应的放大特性。     

A comparison of flow development in high density gas‐solids circulating fluidized bed downer and riser reactors

Comparison of flow development in high density downer and riser reactors is experimentally investigated using fluid catalytic cracking particles with very high solids circulation rate up to 700 kg/m²s for the first time. Results show that both axial and radial flow structures are more uniform in downers compared to riser reactors even at very high density conditions, although the solids distribution becomes less uniform in the high density downer. Solids acceleration is much faster in the downer compared to the riser reactor indicating a shorter length of flow development and residence time, which is beneficial to the chemical reactions requiring short contact time and high product selectivity. Slip velocity in risers and downers is also first compared at high density conditions. The slip velocity in the downer is much smaller than in the riser for the same solids holdup indicating less particle aggregation and better gas‐solids contacting in the downer reactors. © 2015 American Institute of Chemical Engineers AIChE J, 61: 1172–1183, 2015     

气固下行流化床反应器 Ⅲ气、固混合

与气固并流上行提升管反应器相比，气固并流下行管反应器的轴向气固返混明显降低，而径向气固混和仍然相当大，因而有利于提高气固快速反应的转化率及选择性。本文在分析下行流化床反应器内气、固混合机理的基础上，比较了有关气、固混合的研究方法及结果，并比较了提升管和下行管的不同混合现象，旨在促进对这一课题更加深入系统地研究，以适应循环床下行管反应器设计、放大和模型化的迫切要求。     

Analysis of the Particle Clustering Phenomenon in the Fluid Catalytic Cracking of Gasoil in a Downer Reactor

A large eddy simulation (LES)‐discrete element method (DEM) investigation was carried out to study particle clusters in a canonical downer reactor during the fluid catalytic cracking of gasoil. The analysis considered two cases: with and without chemical reactions. The results of the system under cold‐flow conditions for the frequency and mean lifetime of clusters were in good agreement with experimental data. The changes in the hydrodynamic conditions generated by the cracking reactions led to clusters with shorter mean lifetime but higher frequency compared to the system without chemical reactions. Additionally, the frequency and mean lifetime of clusters were successfully correlated to an empirical expression as a function of the particle Reynolds number and the Stokes number, which summarize the hydrodynamic conditions of the downer.     

Modeling of a multizone gas‐phase polyethylene reactor with a cluster‐based approach

A circulating fluidized reactor of polyethylene was modeled with the proper hydrodynamics for a riser and downer and combined with a kinetic model based on the moment equations. The hydrodynamic model was able to predict the profiles of the following parameters through the riser and downer: cluster velocity, bed porosity, concentration of potential active sites, active sites, gas‐phase components, molecular weights, and reactor temperature. It was shown that one could control the monomer consumption and molecular weight, which are crucial in the reactor behavior and production properties, respectively, by setting different operating hydrodynamic conditions, such as the gas velocity in the riser and the solid circulation rate. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Comparisons of particle cluster diameter and concentration in circulating fluidized bed riser and downer using computational fluid dynamics simulation

The information of particle cluster dynamics is necessary for improving the performance of a circulating fluidized bed system. The main objective of this study is to compare the particle cluster diameters and concentrations from computational fluid dynamics simulation results between circulating fluidized bed riser and downer. The calculation methodologies are based on the concept of kinetic theory of granular flow and statistics. The mathematical model was verified by using the experimental dataset from literature and used for computing the particle cluster dynamics. In the circulating fluidized bed riser and downer, a dense and dilute core-annulus flow structures were obtained, respectively. The particle cluster in the circulating fluidized bed riser possessed more heterogeneity movements than that in the circulating fluidized bed downer. This can be explained by the system flow direction. About the particle cluster dynamics, the particle cluster diameters and concentrations in the circulating fluidized bed riser were higher than the ones in the downer. The calculated values were comparable to the empirical correlations. This confirms the validity of the calculation methodologies. Particle cluster dynamics and its example application inside circulating fluidized bed riser and downer were also discussed.     

A Downer Reactor for Short‐time Plasma Surface Modification of Polymer Powders

This paper introduces a plasma reactor for short‐time plasma surface modification of polymer powders. This reactor type, the so‐called plasma downer reactor (PDR), provides a high reaction rate, which is forced by the high gas velocity and high particle dispersion in the plasma. It combines the advantageous characteristics of the downer principle for the fluid dynamics of gas‐solid phases with plasma surface modification. This work demonstrates that a very short plasma exposure time of 0.1 s effectively improves the wettability of HDPE and Co‐PA powders. The water contact angles of HDPE and Co‐PA powder can be reduced to 72° and 76°, respectively. The surface tensions of both polymer powders could be increased by a factor of 2 up to 43 mN/m. Water/polymer suspensions and pastes can be made without tensides.     

Ozone treatment of textile effluents and dyes: effect of applied ozone dose,pH and dye concentration

The ozonation of wastewater supplied from a treatment plant (Samples A and B) and dye‐bath effluent (Sample C) from a dyeing and finishing mill and acid dye solutions in a semi‐batch reactor has been examined to explore the impact of ozone dose, pH, and initial dye concentration. Results revealed that the apparent rate constants were raised with increases in applied ozone dose and pH, and decreases in initial dye concentration. While the color removal efficiencies of both wastewater Samples A and C for 15 min ozonation at high ozone dosage were 95 and 97%, respectively, these were 81 and 87%, respectively at low ozone dosage. The chemical oxygen demand (COD) and dissolved organic carbon (DOC) removal efficiencies at several ozone dose applications for a 15 min ozonation time were in the ranges of 15–46% and 10–20%, respectively for Sample A and 15–33% and 9–19% respectively for Sample C. Ozone consumption per unit color, COD and DOC removal at any time was found to be almost the same while the applied ozone dose was different. Ozonation could improve the BOD₅ (biological oxygen demand) COD ratio of Sample A by 1.6 times with 300 mg dm^?3 ozone consumption. Ozonation of acid dyes was a pseudo‐first order reaction with respect to dye. Increases in dye concentration increased specific ozone consumption. Specific ozone consumption for Acid Red 183 (AR‐183) dye solution with a concentration of 50 mg dm^?3 rose from 0.32 to 0.72 mg‐O₃ per mg dye decomposed as the dye concentration was increased to 500 mg dm^?3. © 2002 Society of Chemical Industry     

提升管与下行床颗粒团聚行为的离散颗粒模拟

从微观机理出发,采用计算流体力学和离散单元方法（CFD-DEM）结合的模型对二维提升管和下行床气固流动体系进行了数值模拟。模拟选用了粒径为520 μm、密度为2620 kg·m-3的球形颗粒和周期性边界条件,展示了气固并流逆重力场和顺重力场运动的颗粒聚团瞬态图像,定性或半定量地揭示了两个不同体系的颗粒微观聚集行为。提升管中颗粒聚团较为严重,且表现明显的颗粒返混现象;下行床中的颗粒聚团比较松散,且具有与宏观流动相同的流速方向,几乎无颗粒返混。通过统计分析获得宏观时均流体力学行为,包括两相的相分布和速度分布,并与文献报道的实验现象进行定性的比较。     

Downer Catalytic Pyrolysis (DCP): A Novel Process for Light Olefins Production

Based on the analysis of different existing cracking processes, the DCP (downer catalytic pyrolysis) process is proposed for the production of light olefins from heavy feeds. A hot downer reactor with the height of 4.5 m and the inner diameter of 13 mm was designed and built to examine the details. The experimental results show that high olefins yields can be obtained from the DCP process: at the temperature of 659 °C and residence time of 0.75 seconds, the total yields of ethylene, propylene and butylene are up to 51.54 wt.‐%, while the methane and coke are suppressed. At the same time, the stability of liquid products is desirable because of the high content of aromatics but low concentration of olefins.     

提升管和下行床在催化裂化过程中的比较

在综合考虑流动、反应、传质的基础上,建立了适用于模拟提升管和下行床反应器中催化裂化过程的二维返混模型,并利用正交配置法进行数值求解,得到了各产物在两种反应器内的不同浓度分布规律。这处结果源于两者流动结构和混合状况的差异。和提升管相比,由于下行床内的气固两相流动更接近平推流,气固速度和颗粒浓度径向分布均匀,气固轴向返混小,因而可得到更高的汽油收率。     

气固并流下行床反应器出入口结构研究现状与展望

自80年代中期以来,气固并流下行床反应器以其接触时间短、接近平推流而成为气固流态化新的研究方向。本文对目前下行床反应器出入口结构方面的研究现状进行了总结,包括下行床出入口结构设计、出入口形式对下行管流动混合行为的影响气固分离效率等。在此基础上,探讨了下行床出入口结构及其性能之间的关系,并提出了下行出入口设计与放大的基本思路。