Different efficiency toward the biomimetic aerobic oxidation of benzyl alcohol in microchannel and bubble column reactors: Hydrodynamic characteristics and gas–liquid mass transfer

The selective aerobic oxidation of benzyl alcohol to benzaldehyde has attracted considerable attention because benzaldehyde is a high value-added product. The rate of this typical gas–liquid reaction is significantly affected by mass transfer. In this study, CoTPP-mediated(CoTPP: cobalt(II) mesotetraphenylporphyrin) selective benzyl alcohol oxidation with oxygen was conducted in a membrane microchannel(MMC) reactor and a bubble column(BC) reactor, respectively. We observed that 83% benzyl alcohol was converted within 6.5 min in the MMC reactor, but only less than 10% benzyl alcohol was converted in the BC reactor. Hydrodynamic characteristics and gas–liquid mass transfer performances were compared for the MMC and BC reactors. The MMC reactor was assumed to be a plug flow reactor,and the dimensionless variance was 0.29. Compared to the BC reactor, the gas–liquid mass transfer was intensified significantly in MMC reactor. It could be ascribed to the high gas holdup(2.9 times higher than that of BC reactor), liquid film mass transfer coefficient(8.2 times higher than that of BC reactor), and mass transfer coefficient per unit interfacial area(3.8 times higher than that of BC reactor). Moreover,the Hatta number for the MMC reactor reached up to 0.61, which was about 15 times higher than that of the BC reactor. The computational fluid dynamics calculations for mass fractions in both liquid and gas phases were consistent with the experimental data.

Hydrodynamics and Mass Transfer in a Modified Three-phase Airlift Loop Reactor

A modified internal-loop airlif reactor （MIALR） with a continuous slurry phase was studied to investigate the local hydrodynamic characteristics, including gas holdup, bubble size, bubble rise velocity and local mass transfer properties. Based on the analysis of geometrical construction and fluid properties of gas and slurry, MIALR was divided into six flow regions. In these flow regions, the local hydrodynamic characteristics were investigated over a wide range of operating variables. Furthermore, a new method was developed to measure the dissolved oxygen concentration. The volumetric mass-transfer coefficient in six flow regions was also calculated for comparison.

Experimental determination of gas holdup and volumetric mass transfer coefficient in a jet bubbling reactor

The hydrodynamics and mass transfer characteristics of a lab-scale jet bubbling reactor(JBR)including the gas holdup,volumetric mass transfer coefficient and specific interfacial area were assessed experimentally investigating the influence of temperature,pH and superficial gas velocity.The reactor diameter and height were 11 and 30 cm,respectively.It was equipped with a single sparger,operating at atmospheric pressure,20 and 40℃,and two pH values of 3 and 6.The height of the liquid was 23 cm,while the superficial gas velocity changed within 0.010-0.040 m·s^(-1)range.Experiments were conducted with pure oxygen as the gas phase and saturated lime solution as the liquid phase.The liquid-side volumetric mass transfer coefficient was determined under unsteady-state oxygen absorption in a saturated lime solution.The gas holdup was calculated based on the liquid height change,while the specific interfacial area was obtained by a physical method based on the bubble size distribution(BSD)in different superficial gas velocities.The results indicated that at the same temperature but different pH,the gas holdup variation was negligible,while the liquid-side volumetric mass transfer coefficient at the pH value of 6 was higher than that at the pH=3.At a constant pH but different temperatures,the gas holdup and the liquid-side volumetric mass transfer coefficients at 40℃were higher than that of the same at 20℃.A reasonable and appropriate estimation of the liquid-side volumetric mass transfer coefficient(kla)in a pilot-scale JBR was provided which can be applied to the design and scale-up of JBRs.

Modeling of mass transfer characteristics of bubble column reactor with surfactant present

Danckwert's method was used to determine the specific interfacial area, a, and the individual mass transfer coefficient, κL, during absorption of CO2 in a bubble column with an anionic surfactant in the carbonate-bicarbonate buffer solution and NaAsO2 as catalyst, the presence of which decreases the specific interracial area and the individual mass transfer coefficient. The specific interfacial area and the individual mass transfer coefficient increase with increasing superficial gas velocity. The specific interfacial area decreases whereas the individual mass transfer coefficient increases with increasing temperature. The results of experiments were used to determine the dependence of a, κL, and κLa on the surface tension, the temperature of the absorption phase, and the superficial velocity of the gas. The calculated results from the correlation were found to be within 10% deviation from the actual experimental results.

Analysis and Measurement of Mass Transfer in Airlift Loop Reactors

Inter-phase mass transfer is important to the design and performance of airlift loop reactors for either chemical or biochemical applications, and a good measurement technique is crucial for studying mass transfer in multiphase systems. According to the model of macro-scale mass transfer in airlift loop reactors, it was proved that the airlift loop reactor can be regarded as a continuous stirred tank reactor for measuring mass transfer coefficient. The calculated mass transfer coefficient on such a basis is different from the volumetric mass transfer coefficient in the macro-scale model and the difference is discussed. To describe the time delay of the probe response to the change of oxygen concentration in the liquid phase, a model taking into account the time constant of response is es-tablished. Sensitivity analysis shows that this model can be used to measure the volumetric mass transfer coefficient. Applying this model to the measurement of volumetric mass transfer coefficient in the loop reactor, results that co-incide with the turbulence theory in the literate were obtained.

Polyethoxylation and polypropoxylation reactions：Kinetics,mass transfer and industrial reactor design

Ethoxylation and propoxylation reactions are performed in the industry to produce mainly non-ionic surfactants and ethylene oxide(EO)–propylene oxide(PO) copolymers.Both the reactions occur in gas–liquid reactors by feeding gaseous EO,PO or both into the reactor containing a solution of an alkaline catalyst(KOH or Na OH).Non-ionic surfactants are produced by using liquid starters like fatty alcohols,fatty acids or alkyl-phenols,while when the scope is to prepare EO–PO copolymers the starter can be a mono-or multi-functional alcohol of low molecular weight.Both reactions are strongly exothermic,and EO and PO,in some conditions,can give place to runaway and also to explosive side reactions.Therefore,the choice of a suitable reactor is a key factor for operating in safe conditions.A correct reactor design requires:(i) the knowledge of the kinetic laws governing the rates of the occurring reactions;(ii) the role of mass and heat transfer in affecting the reaction rate;(iii) the solubility of EO and PO in the reacting mixture with the non-ideality of the reacting solutions considered;(iv) the density of the reacting mixture.All these aspects have been studied by our research group for different starters of industrial interest,and the data collected by using semibatch well stirred laboratory reactors have been employed for the simulation of industrial reactors,in particular Gas–Liquid Spray Tower Loop Reactors.

HYSTERESIS OF GAS-LIQUID MASS TRANSFER IN A TRICKLE BED REACTOR

1 INTRODUCTIONTrickle bed reactors are widely used in the process industry,particularly in petroleumhydroprocessing operations,and have been extensively studied by chemical engineers.In atrickle bed reactor,the gas and liquid flow cocurrently down through the packed bedand undergo chemical reactions.However,there exist multiple hydrodynamic stateswhich correspond to either uniform or,in most cases,nonuniform radial distributionof the gas and liquid flows in the packed section.Moreover,the hydrodynamic state

MASS TRANSFER AND HYDRODYNAMICS IN AN AIRLIFT REACTOR WITH VISCOUS NON-NEWTONIAN FLUID

In an internal loop airlift reactor of 55L working volume,the gas-liquid volumetric oxygenmass transfer coefficient k_Lα,gas holdup ε_G and liquid circulation time t_c were measured with the sol-ution of carboxymethyl cellulose(CMC)to simulate the performance of a reactor with highly viscousbroth.Electric conductivity and oxygen probes were used to measure the local gas holdup,liquidcirculation time and oxygen mass transfer coefficient in the individual sections of the reactor(riser,downcomer and the gas-liquid separating section at the top of the reactor)and the total reactor,respectively.The values of k_Lα for the riser,downcomer and separation sections of the reactor were alsoestimated and compared with that for the total reactor.The results show that,both k_Lα and ε_G in-crease but t_c decreases with increasing gas velocity.Correlations and comparisons with works reportedin the literature are also presented.Data show that the methods developed for k_Lα measurements inthe individual section

Mass Transfer Characteristics of H_2 and CO in Mimicked F-T Slurry Bubble Column Reactor

The equilibrium solubilities,volumetric gas-liquid mass transfer coefficients kLa of H_2 and CO were measured as functions of temperature(298―513 K),pressure(1―3 MPa),superficial gas velocity(0.5―3 cm/s) and solid volume fraction(5%―25%) in liquid paraffin/iron-based catalyst slurry bubble column reactor.The volumetric mass transfer coefficients kLa were obtained by measuring the dissolution rate of H_2 and CO.The influences of the operation conditions,such as pressure,temperature,superficial gas velocity and catalyst concentration on kLa,were investigated.Two empirical correlations were proposed to predict kLa values of H_2 and CO in liquid paraffin/solid particles slurry bubble column reactor.The results showed that the equilibrium solubilities of H-2 and CO increased with an increasing temperature and pressure,and the solubility of CO was greater than that for H_2.It was found that the equilibrium solubility can be expressed by Henry's law.The volumetric mass transfer coefficients of H_2 and CO were of the same order of magnitude,and increased with the increase of pressure,temperature and superficial gas velocity.The presence of solid particles decreased kLa values of both H_2 and CO.

Experimental Study on the Hydrodynamics and Mass Transfer Characteristics of Airlift Loop Reactors (ALR)

The promoting effect of ultrasonic wave on the hydrodynamics and mass transfer characteristics of the airlift loop reactor was studied. The effect of the airlift reactor and ultrasonic wave on the reactor’s gas holdup, liquid circulation velocity, mixing time and overall volumetric mass transfer coefficient respectively with and without the presence of ultrasonic wave is empathetically examined and compared. The experiment has proven that the incorporation of ultrasonic wave has no effect on the gas holdup but has the tendency to gradually decrease the liquid circulation velocity and increase the overall volumetric mass transfer coefficient; the effect on the mixing time is relatively complex. At low gas velocity, low powered ultrasonic wave promotes the radial mixing of fluid; with the increase of ultrasonic power, ultrasonic vibration obstructs the radial mixing of fluid. Therefore, there exists an optimal ultrasonic power. Moreover, the effect of ultrasonic wave on the mixing time gradually decreases with the increase of the superficial gas velocity. Correlations were also proposed for the hydrodynamics and mass transfer characteristics of the reactor.

A Comprehensive Review of the Influence of Heat Exchange Tubes on Hydrodynamic,Heat,and Mass Transfer in Bubble and Slurry Bubble

Bubble and slurry bubble column reactors(BCRs/SBCRs)are used for various chemical,biochemical,and petro-chemical applications.They have several operational and maintenance advantages,including excellent heat and mass transfer rates,simplicity,and low operating and maintenance cost.Typically,a catalyst is present in addition to biochemical processes where microorganisms are used to produce industrially valuable bio-products.Since most applications involve complicated gas-liquid,gas-liquid-solid,and exothermic processes,the BCR/SBCR must be equipped with heat-exchanging tubes to dissipate heat and control the reactor’s overall performance.In this review,past and very recent experimental and numerical investigations on such systems are critically dis-cussed.Furthermore,gaps to befilled and critical aspects still requiring investigation are identified.

水合物快速生成技术及装置

气体水合物技术在天然气固态储运、海水淡化和CO_(2)封存等领域有着广阔的应用前景,水合物快速生成是制约水合物技术应用的关键问题之一;由于对水合物快速生成的研究起步较晚,水合物反应器研制发展尚未成熟,生成速率达不到工业要求。如何提高水合物生成速率,实现水合物的快速生成是实现气体水合物技术应用亟待解决的问题之一。结合水合物的生成机理,分析了制约水合物快速生成的影响因素;回顾了各类水合物快速生成装置的结构和原理,从传质传热角度解析了各类反应器的优缺点,并对未来的研究方向提供几点建议:对有良好应用前景的装置加强改进,逐步扩大规模;结合高科技装备,构建新型反应器;构建一个标准的反应器评价体系。

百千瓦级空间核反应堆屏蔽优化研究

屏蔽体尺寸和重量对空间核反应堆和核动力航天器性能有着重要影响,因而屏蔽设计优化是空间核动力系统设计的关键。本文以JIMO项目反应堆为对象,在铍-碳化硼-钨-氢化锂分层组合屏蔽方案的基础上,考虑到辐照剂量的径向分布,采用蒙特卡罗方法计算了负载处辐照剂量和氢化锂中子剂量,分析了屏蔽设计原理,并提出了分步优化方法以实现屏蔽优化。根据结果分析,调整了铍和碳化硼的厚度比例、钨半径及布置位置,获得了优化的屏蔽方案,在满足屏蔽要求的基础上质量减少了98.41 kg。提出的屏蔽方案及设计流程可为空间核电源屏蔽设计优化提供参考。

中空纤维膜臭氧接触式反应器传质机理分析

将疏水性聚四氟乙烯(PTFE)中空纤维膜组装成膜接触器,开发了膜接触式臭氧(O_(3))传质技术。对比了气泡传质和膜接触传质的差异,通过O_(3)传质模型和阻力模型对该技术的主要影响因素和传质机理进行了研究。结果表明,O_(3)可以有效地通过疏水性PTFE膜进行传质,当搅拌速度达到1500r/min时,膜传质的表观传质系数(0.3049min-1)与气泡传质(0.3109min-1)相当。同时,膜表面的疏水结构将尾气的湿度降低到0.8g/m^(3)以下,远低于气泡传质(>11.5g/m^(3)),符合进入臭氧发生器的标准,具备回收氧气的可行性。O_(3)的传质通量受液体流速、p H、污染物浓度、气体流量以及进气O_(3)浓度的影响。在pH=11、苯酚浓度为0或pH=7、苯酚浓度为20mg/L时,传质通量达到了0.16g/(m^(2)·h)。O_(3)传质过程的传质阻力主要由膜阻力和液相阻力组成,而通过液相条件控制可以有效减小液相阻力,因此进一步降低传质阻力需要膜技术的发展。

液态金属堆内小长径比同轴双层薄壁结构的流固耦合试验研究

池式液态金属堆的主容器与热屏之间具有狭窄的流体间隙,该结构属于含窄缝间隙的小长径比同轴双层柔性壳体。窄缝间隙中流体与结构之间相互作用产生的流固耦合效应在抗震分析时必须加以考虑。现有研究主要针对长径比较大和流体间隙相对较大的圆柱壳体,对于小长径比和极小流体间隙的同轴柔性壳体研究较为缺乏。本文参考液态金属反应堆的结构设计了三种不同尺寸的窄缝间隙,开展窄缝间隙条件小长径比同轴双层壳体模型的振动试验,测量结构在不同间隙尺寸下的加速度,得到模态频率和主要振型。然后,使用有限元法进行模态分析,通过与试验结果的对比,验证了有限元法的准确性。最后,计算出不同间隙尺寸下模型的附加质量;且随着间隙尺寸的减小,模型附加质量随之增大。本研究可为类似的含窄缝小长径比同轴双层柔性壳体结构的抗震设计提供数据支持,对于液态金属堆的抗震分析具有重要意义。

低冷量下强化CO_(2)吸收的甲醇基纳米流体性能

冷甲醇洗法捕集CO_(2)技术要求低温环境,需要大量的冷冻能量,能耗较大。在吸收剂中引入纳米颗粒,可以有效提高气液传质速率,降低能耗。本研究旨在开发冷量需求少,吸收、解吸性能提升的甲醇基纳米流体。实验分别考察了纳米颗粒种类、固含量、尺寸,表面活性剂含量、操作温度和初始CO_(2)浓度等因素对吸收剂捕集CO_(2)性能的影响及机理。结果表明,在0.2~1.0g/L的TiO_(2)、Al_(2)O_(3)、SiO_(2)纳米流体中,0.4g/L的TiO_(2)-甲醇纳米流体的CO_(2)吸收、解吸增强效果最佳。向其中添加0.10%(质量分数)聚乙二醇辛基苯基醚(Triton X-100)后,纳米流体的吸收、解吸增强效果达到最大,且在5次循环后仍呈现良好增强效果。此外,本文对纳米流体增强吸收的机理进行了深入分析,提出了一个经验公式来预测TiO_(2)-甲醇纳米流体的增强因子E和最佳固含量。

新型管式搅拌反应器的气液传质特性

多相体系的混合与传质性能直接影响多相反应过程,团队开发了从搅拌桨叶端出气的新型管式搅拌反应器。采用稳态亚硫酸盐法(FSM)研究反应器的气液传质性能,考察了通气流量Q、搅拌弗劳德数Fr和液含量ε对体积传质系数k_(L)a的影响。结果表明:增大Q和Fr可以有效提高k_(L)a;新型搅拌桨从桨叶端进气方式可以增强k_(L)a,相较传统反应器最大增强约2倍。反应器的气液传质性能在ε=0.5、Fr=0.054、Q=1.6 m^(3)·h^(-1)时最高,此时k_(L)a=0.032 4 s^(-1)。依据试验数据建立了关于k_(L)a的无量纲关联式,误差基本在25%以内,对后续反应器的改进和应用具有参考意义。

多孔板鼓泡塔流动与传质特性数值模拟

采用Euler-Euler双流体模型对安装不同数量的水平多孔板的鼓泡塔内气液两相流动及传质特性进行数值模拟研究,并探究了不同表观气速条件对鼓泡塔内气含率、气泡直径分布和气液传质系数的影响。结果表明,不同数量的多孔板和不同位置的多孔板都会影响气含率的分布;随着多孔板的数目增加,鼓泡塔液相上方区域的气含率增加,但影响区域有限;安装多孔板后,鼓泡塔内径向位置的平均气含率变化明显,出现“M”形状的分布。不同表观气速下,未安装多孔板的鼓泡塔内直径为1~2mm的微小气泡占比超过30%;安装多孔板后,微小气泡占比明显增加;气液传质系数在中心区域(径向无量纲为-0.5~0.5)较为平缓,波动不大。最后将模拟计算得到的气液体积传质系数与Akita的关联式计算值进行比较,本文计算结果略高。

A convenient method for measuring gas-liquid volumetric mass transfer coefficient in micro reactors

The research on gas-liquid multiphase reactions using micro reactors is becoming increasingly widespread, given their excellent mass transfer performance. Establishing an accurate and reliable method to measure the gas-liquid mass transfer performance of micro reactors is crucial for evaluating and optimizing the design of micro reactor structure. In this paper, the physical absorption method of aqueous solution-CO_(2) and the chemical absorption method of sodium carbonate solution-CO_(2) were proposed. By analyzing the chemical reaction equilibrium during the absorption process, the relationship between the mass transfer of CO_(2) and the solubility of hydroxide ions in the solution was established, and the total gas-liquid mass transfer coefficient was immediately obtained by measuring the p H value. The corresponding testing platform and process have been established based on the characteristics of the proposed method to ensure fast and accurate measurement. In addition, the chemical absorption method takes into account temperature factors that were not previously considered. The volumetric mass transfer coefficient measured by these two methods is in the same range as those measured by other methods using the same microchannel structure in previous literature. The methods have the advantages of low equipment cost, faster measurement speed, and simpler procedures, which can facilitate its wide application to the evaluation of the mass transfer performance and hence can guide the structure optimization of microchannel reactors.

小型堆中窄矩形通道自然循环临界热流密度实验研究

针对窄矩形通道在换热过程中有较高功率密度的问题,本文为了解决在小型反应堆中的应用,采用所搭建的小型窄矩形自然循环通道,进行实验研究,并结合BP神经网络方法对实验数据进行预测,分析在不同参数工况下临界热流密度随不同参数的变化情况以及不同参数对临界热流密度的影响程度。研究结果表明:质量流量与系统压力对临界热流密度点的影响呈现正相关;出口干度对临界热流密度呈现负相关;且质量流量对临界热流密度的影响程度最大;压力对临界热流密度的影响程度最小。利用相关实验数据,基于影响因素大小,通过BP神经网络方式,建立了适合于自然循环窄通道小堆的模型。BP神经网络算法的预测值与实验值符合良好,误差为10%;Katto模型与实验数据相比误差较大,Zhang公式和拟合公式的误差较小,所建立的临界热流密度模型可作为窄矩形通道自然循环临界热流密度的计算公式。