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     

Mass transfer and selectivity of ozone reactions

The present research concerns the behavior of mass transport in absorption of ozone accompanied by decomposition and ozonation reactions in aqueous solutions. On the basis of the film theory, a mathematical model has been formulated for the transport process taking into account molecular diffusion and the simultaneous decomposition and ozonation reactions of different orders. Analytical approximate and finite difference methods have been employed to predict concentration profiles, enhancement factor and selectivity of the chemical mass transfer in gas-liquid systems. The rate of mass transfer is enhanced by the chemical reactions as well as the availability of liquid reactant in the aqueous phase. When the ozonation reaction is much faster than the decomposition reaction, a large fraction of the absorbed ozone is utilized effectively in reacting with the liquid constituent and a high selectivity of the gas-liquid reactions can be obtained. Calculated results indicate that removal of certain organic pollutants by the oxidation process may be effective only in acidic or neutral solutions where a high mass transfer rate and selectivity is achieved.     

亚硫酸盐强制氧化传递与化学反应动力学

在湿法烟气脱硫的过程中,吸收塔底部发生的反应主要是亚硫酸钙和空气或氧气之间的气液传递与化学反应过程,根据双膜理论模型,分析了该反应的吸收机理,用一种图像边界识别的方法分析亚硫酸盐强制氧化气液反应.在没有催化剂或固定钴离子催化剂浓度时,SO^2-₃存在临界浓度0.328 mol•L^-1.当SO^2-₃的浓度低于0.328 mol•L^-1时,过程为双膜控制,SO^2-₃的反应级数为1;当SO^2-₃的浓度大于0.328 mol•L^-1时,过程逐渐变为气膜控制,SO^2-₃反应级数为0.当固定SO^2-₃浓度时,催化剂钴离子的反应级数则受到气液传质的影响,分为几个阶段,且反应级数不同.     

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.     

Numerical modeling of mass transfer processes coupling with reaction for the design of the ozone oxidation treatment of wastewater

A computational model for an ozone oxidation column reactor used in dyeing wastewater treatment is proposed to represent, simulate, and predict the ozone bubble process. Considering the hydrodynamics, mass transfer, and ozone oxidation reaction, coupling modeling can more realistically calculate the ozone oxidation bubble process than the splitting methods proposed in previous research. The modeling is validated and shows great consistency with experimental data. The verified model is used to analyze the effect of operating conditions, such as the initial gas velocity and the ozone concentration, and structural conditions, such as multiple gas inlets. The ozone consumption is influenced by the gas velocity and the initial ozone concentration. The ozone’s utilization decreases with the increasing gas velocity while nearly the same at different initial ozone concentrations. Simulation results can be used in guiding the practical operation of dyeing wastewater treatment and in other ozonation systems with known rate constants in wastewater treatment.     

基于电渗析的溶液再生传质模型及性能分析

电渗析溶液再生与传统热再生相比具有较大的节能潜力,近年来受到了越来越多的关注。目前有关电渗析溶液再生的研究主要都集中在系统层面的分析,而缺乏对电渗析传质机理的认识。为此,建立了描述电渗析在高浓度下的传质理论模型,并试验探究了不同电流密度、体积比及初始浓度对系统性能的影响。结果表明,模型和试验结果吻合很好,误差小于±4%。体积比越大时,系统再生性能越好,但溶液产量也越低;电流密度越大时,系统再生性能越好,但系统能耗也越高;初始浓度越高时,系统电流效率和再生性能越低,同时膜堆中浓差极化系数也越低。在实际应用时应权衡以上因素以实现更高的系统性能和效率。     

Mass transfer and reaction of trimethylamine in a three-phase biological reactor

A model system, consisting of a mixed culture of microorganisms, was used to study the performance of a bench-scale packed bed bubble column (PBC) bioreactor treating trimethylamine. Three mesophilic bacterial strains were selected, mixed and acclimatized to grow with trimethylamine as the sole carbon source; degradation kinetic constants were determined for a bacterial suspension system. Gas transfer to the liquid phase was modelled in order to characterize solute transport and availability into the biofilm. The overall performance of the system is discussed based on mass transfer considerations.     

Mass transfer and hydrodynamic characteristics in a co‐current downflow contacting column

Hydrodynamic and mass transfer characteristics of water–air system in a co‐current downflow contacting column (CDCC) were studied for various nozzle diameters at different superficial gas velocities and liquid re‐circulation rates. Gas hold‐up and liquid‐side mass transfer coefficient increased with increasing superficial gas velocity and liquid flow rate but decreased with increasing nozzle diameter. It is shown that correlations developed, which are based on liquid kinetic power per liquid volume present in the column, and superficial gas velocity explains gas hold‐up and the mass transfer coefficient within an error 20% for all gas and liquid flow rates and nozzle diameters used. The constants of correlations for gas hold‐up and mass transfer coefficient were found to be considerably different from other gas–liquid contacting systems. © 2003 Society of Chemical Industry     

下行床反应器热试装置设计与开发

气固并行向下流动的下行床反应器比提升管具有气固接触时间短、气固速度及浓度径向分布更为均匀、气固轴向返混大大减少、易实现高固气比操作等特点。在下行床反应器小型热试装置开发过程中,为发挥下行床的技术优势,重点研究和解决了反应器出入口结构、原料雾化、高温高流通量下固体循环量测量与控制等几个关键性的工程问题,为下行床反应器的热试研究和应用开发提供了基础。     

臭氧吸收及反应过程的传质系数与增强因子

从双膜理论、溶质渗透理论、膜－渗透理论和表面更新理论出发，研究分析了臭氧气体在液相中的物理吸收过程传质系数，臭氧与液相中的污染物化学反应过程的吸收系数。基于双膜模型理论，推导出在不同pH值区间内伴随着臭氧与污染物化学反应过程的增强因子表达式。     

旋流气液两相强化吸收CO2的传质性能

为强化二氧化碳的吸收过程,采用一类旋流逆向气液多级接触的方式,以NaOH溶液为吸收剂,研究其与大跨度浓度CO₂(2.5%～15%)接触反应的传质性能。分别探讨了吸收剂浓度、吸收剂流量、烟气CO₂浓度、烟气流量及反应温度对气相总体积传质系数(K_ga)的定量影响。结果表明,在实验条件下,其K_ga可达(4.53×10^-5)～(9.22×10^-5)kmol·m^-3·s^-1·kPa^-1。与双级直流喷雾和单级旋流喷雾相比,旋流逆向气液多级接触能够有效强化大跨度浓度CO₂的吸收过程。K_ga随吸收剂浓度、流量和反应温度的增加而增加,随CO₂浓度增加呈现先增加后减小(CO₂浓度大于5%)的非线性关系,随气体流量增加先增加后趋于稳定。     

多层搅拌式生物反应器内冷模和热模的传质特性

采用不同浓度的羧甲基纤维素钠（CMC）溶液替代菌丝发酵液进行两种桨型组合（三层平直叶圆盘涡轮,3PY和底层半圆管圆盘涡轮HY及上面两层三宽叶翼型轴流桨KCXu,HY+2KCXu）的功率消耗和体积氧传质系数研究。结果表明：相同功率下,低浓度CMC溶液中上翻操作的HY+2KCXu组合的传质能力更好,但是随着黏度的增加,两种组合的传质能力趋于相同。同时采用两种桨型组合进行黑曲霉产糖化酶的发酵实验,通过调节转速实现两种桨型下发酵罐内菌体的氧摄取速率相近,通过对产酶量、菌形、发酵液流变特性以及反应器内的传质能力对比研究发现：发酵过程中装有HY+2KCXu组合的罐内发酵液的表观黏度低于装有3PY组合的罐,HY+2KCXu罐内似乎更容易形成菌球,菌球的形成降低了发酵液的黏度,传质系数增大,从而提高了产酶效率。     

Mass transfer variation within a packed bed and its relation to liquid distribution

The limiting current method is applied to characterize the local mass transfer in the axial, radial and angular directions throughout a packed bed of Pall rings. This is expressed in terms of the particle-to-fluid mass transfer coefficient of ferricyanide ions obtained from the limiting currents measured during its reduction to ferrocyanide at different locations in the bed. Particular focus is placed on the variability of the mass transfer coefficient with position in terms of the quantity MT_VAR, equivalent to the normalized deviation of the function Sh/Sc^0.33. The results confirm those reported by other researchers using more traditional liquid collection and tracer methods. Mass transfer coefficients throughout the bed closely follow normal distributions for the range of Re values investigated. When a multipoint distributor is used, MT_VAR is already low at the lowest flow rate (Re=95) considered and remains unchanged with any further increase in flow rate. In the case of a single-point distributor, on the other hand, MT_VAR decreases with increasing flow rate, but always remains significantly higher than that observed with the multipoint distributor. Moreover, the MT_VAR value depends on whether irrigated or full flow conditions prevail and on the cross-sectional area of the sampling electrodes, suggesting that local mass transfer variations are caused by local liquid velocity variations once the Pall rings are sufficiently wetted.     

Mass transfer between solid particles and liquid in a three phase fluidized bed

Particle-liquid mass transfer in a co-current three-phase fluidized bed of glass beads, water and air was studied with two measurement techniques. Both techniques measured the weight loss of a few particles coated with benzoic acid in a bed of inert glass beads. The effects of liquid and gas velocities, gas distribution and surface active agents on particle-liquid mass transfer in a three-phase fluidized bed were thus determined. In the absence of surface active agents in the liquid, particle-liquid mass transfer rates in a three-phase fluidized bed were up to 30% higher than in the corresponding liquid fluidized bed. When surface active agents were added to the liquid, the particle-liquid mass transfer rate was increased by up to about 100% in the three-phase fluidized bed, relative to the liquid fluidized bed. The particle-liquid mass transfer coefficient was found to be inversely proportional to the liquid hold-up in the three-phase fluidized bed.     

微通道内二乙醇胺/乙醇溶液吸收CO2的传质性能

利用高速摄像仪实验研究了微通道内二乙醇胺（DEA）/乙醇溶液吸收CO₂的传质过程。采用图像法得到微通道内气泡的体积变化,根据微通道进出口压力,计算得到了气液两相从开始接触到平衡时的平均传质系数k。分别考察了气液相流量和DEA浓度对传质系数的影响。结果表明：传质系数随着液相流量和溶液中DEA浓度增大而增大。对于给定的液相流量和DEA浓度,k随着气相流量增大而增大并逐渐趋于一个恒定值。提出了一个传质系数预测式,预测值和实验结果吻合良好。     

Mass transfer and substrate utilization in biofilm reactors

Mass transfer within microbial films is described using Monod-type biological kinetics in terms of properties of packing material and the feed solution. For this purpose, computer techniques have been developed for the numerical evaluation of the normalized biofilm mathematical model. A second-order partial differential equation, describing the mechanisms of dispersion phenomena inside the liquid layer, was then solved to determine the mass transfer coefficient. The application of the theory to earlier experimental data has also been demonstrated.     

双搅拌釜中半胱氨酸亚铁溶液吸收NO的传质-反应动力学

以半胱氨酸亚铁络合物Fe(Ⅱ)(CyS)₂作为吸收剂,在双搅拌釜内探讨了NO吸收反应动力学.实验结果表明：在pH=8.0,T=323 K实验条件下,半胱氨酸亚铁溶液吸收NO气体为快速拟一级反应,得到二级反应速率常数k₂=1.18×10⁵ m³•mol^-1•s^-1.3种理论模型即膜模型、Danckwerts表面更新模型、Higbie渗透模型应用于该拟一级反应,增强因子的计算结果是相同的.实验获得的增强因子与模型计算值吻合较好,最大相对偏差不超过13％.     

电场强化臭氧向水中传质的试验研究

首次提出了利用电场强化臭氧向水中传质过程的方法,结果表明:电场能够强化臭氧向水中的传质过程,而且效果和电场的强弱有关,试验中所加电压越高,对于传质的加强效果越明显。当电压为8kV时,和没有电场的情况相比,总传质系数提高41%。该方法为研究臭氧向水中的传质提供了新的途径。