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。     

格子Boltzmann方法模拟咸水吸收CO2的Rayleigh对流过程

由溶解的CO₂引发的Rayleigh对流,对咸水层中CO₂的捕获与封存至关重要。为了更加直观地了解该过程的混合规律和盐浓度变化带来的影响,本文采用格子Boltzmann方法（LBM）对该过程进行了模拟。通过建立包含密度和浓度分布函数的双分布模型,同时引入静电力和体积力等外力项,对293.15K、101kPa下有多个离散的CO₂扩散源时的浓度分布进行了模拟。结果表明,模拟得到的Rayleigh对流结构、对流发生时间、流场速度和瞬时传质通量的数量级与前人研究结果一致;在咸水吸收CO₂过程中,Rayleigh对流结构可有效强化传质;瞬时传质通量随着时间增长先减小后增大再减小,对应了Rayleigh对流结构产生、发展、稳定的变化过程。同时模拟CO₂在纯水和不同盐浓度咸水中的溶解过程结果表明,盐浓度的增加会延迟Rayleigh对流的开始时间、降低传质效率,这与前人的实验结果一致,模拟结果可为不同盐浓度咸水层中CO₂的封存提供指导。     

SIMULTANEOUS ABSORPTION OF H2S AND CO2 INTO A SOLUTION OF SODIUM CARBONATE

The simultaneous absorption of H₂S and CO₂ has been studied both experimentally and theoretically. A model has been developed which predicts the absorption rates of H₂S and CO₂ into a sodium carbonate solution. The absorption rates are calculated according to the two-film theory. In the liquid film, the finite rate of the CO₂ reaction was considered. Otherwise, in the liquid film as well as in the liquid bulk, equilibrium conditions for all reactions were assumed. Absorption experiments were performed on a packed column using a counter-flow strategy. In the experiments the influence of the initial carbonate concentration, the gas flow rate and the temperature on the removal efficiencies of H₂S and CO₂ and the selectivity of H₂S were investigated. It is desirable to absorb the H₂S but not the CO₂. The agreement between the absorption model and the experimental results from the absorber tower was satisfactory. The mass transfer coefficients were determined by fitting the experimental data to the model with respect to the H₂S and CO₂ content in the outgoing gas. The H₂S content was used to determine the gas side mass transfer coefficient and the CO₂ content was used to determine the liquid side mass transfer coefficient, The effective contact area of mass transfer was taken from published data. With a constant packing height, both the experiments and the model indicated that high carbonate concentration benefits the removal efficiency of H₂S. Higher gas flow rate also benefits the selectivity for H₂S. However, the removal efficiency will decrease. At higher temperatures the selectivity and the removal efficiency of H₂S decreased. Under the conditions investigated, the absorption of H₂S was essentially controlled by gas-side mass transfer and the absorption of CO₂ was controlled by liquid-side mass transfer     

富氧燃烧烟气冷凝塔钠碱法脱硫过程SO2和CO2共吸收建模与实验研究

建立SO₂与CO₂共吸收到钠基溶液中的吸收速率模型,假设该模型中SO₂的水解反应为瞬间反应;关于CO₂水解反应存在两种假设：有限动力学假设和瞬间反应假设。由这两种方法计算分别获得SO₂的吸收速率并与完全预混气液反应器中的的动态实验进行对比。采用瞬间反应假设可以预测反应速率的趋势,绝对反应速率误差仍然较大。而采用有限动力学假设的模拟值与实验值在pH>3吻合良好。CO₂对SO₂吸收速率的影响主要通过影响气相传质系数和相同pH下溶液总硫浓度产生。根据CO₂存在与否对SO₂吸收速率的影响,获得五个不同的相互作用pH的区间。pH>11.42时,SO₂/N₂吸收速率大于SO₂/CO₂,主要由于气相传质系数影响;7.8 < pH < 11.42时,SO₂/N₂的吸收速率和SO₂/CO₂吸收速率相似,主要由于气相传质系数和溶液总硫影响抵消;5.41 < pH < 7.8时,SO₂/CO₂的吸收速率相对较高,主要由于溶液总硫影响更大;2.8 < pH < 5.41时,SO₂/CO₂的吸收速率相对较低,主要由于气相传质系数影响;pH < 2.8时,SO₂/N₂和SO₂/CO₂吸收速率相似,主要受液相传质的控制。模拟同时获得不同pH下溶液中碳和硫相关离子的转化规律和SO₂吸收速率的控制步骤,为富氧燃烧冷却塔同时脱硫设备的设计和运行提供参考。     

Performance of CO2 absorption in a diameter-varying spray tower

The application of spray towers for CO₂ capture is a development trend in recent years. However, most of the previous jobs were conducted in a cylindrical tower by using a single spray nozzle, whose configuration and performance is not good enough for industrial application. To solve this problem, the present work proposed a diameter-varying spray tower and a new spray mode of dual-nozzle opposed impinging spray to enhance the heat and mass transfer of CO₂ absorption process. Experiments were performed to investigate the mass transfer performance (in terms of the CO₂ removal rate (η) and the overall mass transfer coefficient (K_Ga_e2 are major factors, which affect the absorption performance and the maximums of η and K_Ga_e that are 94.0% and 0.574 kmol·m^-3·h^-1·kPa^-1, respectively, under the experimental conditions. Furthermore, new correlations to predict the mass transfer coefficient of the proposed spray tower are developed in various CO₂ concentrations with a Pearson Correlation Coefficient over 90%.     

CO2 absorption performance in a rotating disk reactor using DBU-glycerol as solvent

Gas–liquid mass transfer of rotating disk reactor was studied in CO_2 absorption using 1,8-diazabicyclo-[5.4.0]-undec-7-ene(DBU)-glycerol solution as solvent. Effects of the rotating disk structure and various operation parameters on the CO_2 absorption rate and CO_2 removal efficiency were investigated. The rotating disk with optimal holes is conducive to mass transfer of CO_2 and the formation of thin liquid film at the opening increases the gas–liquid contact area. With the increase of rotating speed, the liquid flow pattern on the rotating disk surface changes from thin film flow to separated streams and creates extra liquid lines attached to the rim of the disk,which leads to a very complicated change on the CO_2 absorption rate and CO_2 removal efficiency. The overall gas-phase mass transfer coefficient increases 138% as the rotating speed increasing from 250 to 1400 r·min~(-1).Increasing temperature from 298 to 338 K can enhance the CO_2 absorption rate due to lowering the viscosity of the solvent. The rate-determined step for the absorption is focused on the gas side. The rotating disk reactor can effectively enhance the absorption of CO_2 with viscous DBU-glycerol solvents.     

阵列凸起微通道内气液两相传质特性研究

研究了阵列凸起微通道内N-甲基二乙醇胺（MDEA）吸收CO₂过程的气液两相传质特性。在弹状流型下,考察了气液两相流量、MDEA浓度对体积传质系数、CO₂吸收效率、压力降以及能量损耗的影响。弹状气泡受到阵列凸起的挤压作用发生形变,促进了气液两相间的传质。与平滑通道相比,阵列凸起微通道在实验条件下具有更好CO₂吸收效率。在相同的能量损耗时,阵列凸起微通道具有更大的体积传质系数。     

Experimental study of the mass transfer behavior of carbon dioxide absorption into ternary phase change solution in a packed tower

Phase change absorbents for CO₂ are of great interest because they are expected to greatly reduce the heat energy consumption during the regeneration process. Compared with other phase change absorbents, monoethanolamine (MEA)-sulfolane-water is inexpensive and has a fast absorption rate. It is one of the most promising solvents for large-scale industrial applications. Therefore, this study investigates the mass transfer performance of this phase change system in the process of CO₂ absorption in a packed tower. By comparing the phase change absorbent and the ordinary absorbent, it is concluded that the use of MEA/sulfolane phase change absorbent has significantly improved mass transfer efficiency compared to a single MEA absorbent at the same concentration. In the 4 mol·L^-1 MEA/5 mol·L^-1 sulfolane system, the CO₂ loading of the upper liquid phase after phase separation is almost zero, while the volume of the lower liquid phase sent to the desorption operation is about half of the total volume of the absorbent, which greatly reduces the energy consumption. This study also investigates the influence of operating parameters such as lean CO₂ loading, gas and liquid flow rates, CO₂ partial pressure, and temperature on the volumetric mass transfer coefficient (K_Ga_V). The research shows that K_Ga_V increases with increasing liquid flow rate and decreases with the increase of lean CO₂ loading and CO₂ partial pressure, while the inert gas flow rate and temperature have little effect on K_Ga_V. In addition, based on the principle of phase change absorption, a predictive equation for the K_Ga_V of MEA-sulfolane in the packed tower was established. The K_Ga_V obtained from the experiment is consistent with the model prediction, and the absolute average deviation (AAD) is 7.8%.     

水力喷射-空气旋流器中气液传质特性及其机理

对一种新型高效的气液传质设备--水力喷射-空气旋流器(WSA)的传质机理进行了研究。分别采用化学吸收法(CO₂-空气-NaOH体系)和物理吸收法(CO₂-空气-H₂O体系)测定了不同进口气速、不同液体喷射速度下的有效相界面积a和液膜传质系数k_L,并由此得到体积传质系数k_La。结果表明,由于WSA中气液间的强交互作用,a、k_L以及k_La均随进口气速和液体喷射速度增大而增大。采用量纲分析法对实验数据进行了归纳,拟合出了a、k_L和k_La随气相Reynolds数Re_g、液相Weber数We_L之间的经验公式:a=0.0024Re_g^1.25We_L^0.079,Sh_L=35.31Re_g^0.2303We_L^0.13,k_La=6.52×10^-8Re_g^1.48We_L^0.21,这些关联式能较好地预测WSA的传质性能。研究还表明,在WSA中的气液射-旋流传质体系中,传质过程符合双膜理论、表面更新理论和溶质渗透理论,但以表面更新机理为主。     

三维菱形结构微通道内气液传质与强化

研究了具有三维交错菱形结构的微通道对离子液体1-丁基-3-甲基咪唑四氟硼酸盐([Bmim][BF₄])水溶液吸收CO₂过程的传质增强作用。实验主要聚焦于弹状流和破碎弹状流。考察了弹状流型下气液流量、离子液体浓度对体积传质系数k_La、增强因子E、CO₂吸收率X及压力降ΔP的影响。结果表明,较之于直通道,三维菱形通道可以显著提高体积传质系数和CO₂吸收率,其增强因子可达2.1,压力降仅增加 0.9 kPa。提出了一个新的体积传质系数k_La预测式,预测效果良好。采用VOF法模拟了微通道内气液两相流动过程,获得了连续相的速度矢量场。三维菱形通道能诱导涡流,强化传质过程。     

Mass transfer correlations for membrane gas-solvent contactors undergoing carbon dioxide desorption

Membrane gas-solvent contactors are a hybrid technology combining solvent absorption with membrane gas separation, which demonstrates potential for CO₂ capture through the ability of the membrane to rigidly control the mass transfer area. Membrane contactors have been successfully demonstrated for CO₂ absorption, and there is strong research interest in using membrane contactors for the complimentary CO₂ desorption process to regenerate the solvent. However, understanding and modelling the various stages of mass transfer in the desorption process is less well-known, given the existing mass transfer correlations had been developed from absorption experiments. Hence, mass transfer correlations for membrane contactors are reviewed here, and their appropriateness for desorption analysed. This is achieved through simulating CO₂ desorption through a membrane contactor from loaded 30wt% monoethanolamine solvent to enable comparison of the correlations. It was found that the most cited correlations by Yang and Cussler were valid for shell side parallel flow, while that of Kreith and Black was viable for shell side cross flow. A limitation of all of these correlations is that they assume single phase flow on both sides of the membrane; however, the high temperature of CO₂ desorption can lead to partial solvent vaporisation and hence two phases present on one side of the membrane contactor during desorption. A mass transfer correlation is established here for two phase parallel flow on the shell side of a membrane contactor, based on experimental results for three composite and one asymmetric hollow fibre membrane contactors stripping CO₂ from loaded MEA at 105-108℃. This correlation is comparable to that reported in the literature for mass transfer in other two phase systems, but differs from the standard format for membrane contactors in terms of the exponent on the dimensionless Schmidt and Reynolds numbers.     

微通道内乙醇胺吸收CO2的过程特征（英文）

Process characteristics of CO2 absorption using aqueous monoethanolamine(MEA) in a microchannel reactor were investigated experimentally in this work.A T-type rectangular microchannel with a hydraulic diameter of 408 μm was used.Operating parameters,i.e.temperature,pressure and molar ratio of MEA to CO2 were studied.Under 3 MPa pressure,the mole fraction of CO2 in gas phase could decrease from 32.3% to 300×10?6 at least when gas hourly space velocity ranged from 14400 to 68600 h?1 and molar ratio of MEA to CO2 was kept at 2.2.In particular,the effects of temperature on CO2 absorption flux,mass transfer driving force,gas-liquid contact time and en-hancement factor were analyzed in detail and found that mass transfer enhancement by chemical reaction was a crucial factor for the process of CO2 absorption.     

中空纤维膜接触器脱碳和传质性能的数值研究

中空纤维膜吸收烟气中CO₂是一种清洁、高效、最具潜力的脱碳技术方法之一。本文建立了一个二维的中空纤维膜接触器平行逆流吸收混合气中CO₂的非润湿模型。考虑轴向和径向扩散,模拟了EEA、EDA和PZ 3种吸收剂在不同操作条件下对CO₂的脱除效果和传质性能。结果表明：脱碳性能从大到小为PZ>EDA>EEA;气相参数对脱碳和传质的影响比液相参数更显著;提高气体流速、CO₂浓度和气温,脱碳率均会下降;提高液速、吸收剂浓度和液温,脱碳率均增大,而传质速率只有在提高气温时会下降,其他参数的升高均会使其增大;应采用适当的液相参数,防止操作参数过高带来的不利影响。     

微通道内单乙醇胺水溶液吸收CO2/N2混合气的传质特性

采用高速摄像仪对400 μm×400 μm T形微通道内单乙醇胺（MEA）水溶液吸收混合气中CO₂过程的气液两相流及传质特性进行了实验研究,微通道内的压力降采用压力传感器进行测量。考察了弹状流型下气液两相流量及MEA浓度对压力降、比表面积和传质性能的影响。结果表明,当MEA浓度不变,气液两相流量增大时,压力降、比表面积、传质系数、体积传质系数和增强因子均增大,并逐渐趋于恒定。当气液流量不变,MEA浓度增大时,压力降、传质系数、体积传质系数和增强因子增大,但比表面积减小。实验条件下,压力降范围为2.00~5.23 kPa,化学吸收过程的传质系数范围为7.74×10^-4~2.97×10^-3 m·s^-1。对于伴有快速化学反应的传质过程,以Sherwood数、Reynolds数、Schmidt数及增强因子为变量建立了体积传质系数的预测关联式,平均偏差为5.09%,具有良好的预测性能。     

NaOH-CO2体系下并流立体旋流筛板塔传质性能

二氧化碳捕集是应对全球气候变暖问题的重要技术之一。本文使用NaOH溶液和CO₂作为实验体系,在并流塔中对立体旋流筛板（TRST）的传质性能进行实验研究,测定并计算出全塔及塔板段的气相总体积传质系数[K_Ga_e,(K_Ga_e)_t],重点考察塔板安装数量和方式、空塔气相动能因子和喷淋密度、CO₂和NaOH浓度等参数的影响规律。研究结果表明,塔板段是传质过程的主要区间,增加塔板数量以及采用塔板逆向安装方式是提升传质性能的有效技术手段;塔板段的气相总体积传质系数随空塔气相动能因子和NaOH浓度的增加呈先增大后减小的趋势,随喷淋密度和CO₂浓度的增加而减小,最高可达12.18kmol/(m³·h·kPa);建立塔板段的气相总体积传质系数的经验模型,模型计算值与实验数据的吻合性较好,相对误差小于20%。     

磁场对氨水吸收烟气中CO2的促进作用

开发了一种新型磁场辅助氨法烟气脱碳技术。含碳烟气通入混有磁性颗粒的氨水溶液,在外加磁场的作用下发生脱碳反应。对该技术的运行特性开展了实验研究。结果表明,外加8 mT恒稳磁场,2 g·L^-1纳米级Fe₃O₄颗粒,氨水的CO₂脱除效率比不添加磁场和颗粒时最多可提高8.8%。外加磁场可以有效提高低浓度氨水的CO₂脱除效率。在模拟烟气流量增加时,外加磁场能有效减缓CO₂脱除效率下降的趋势。同时,外加磁场使得CO₂脱除效率曲线向低温方向移动5℃,有助于提高低温条件下的CO₂脱除效率。磁场可提高气液接触效率、降低相间传质阻力、增强氨水反应活性,从而提高氨水吸收CO₂性能。     

CO2在正戊醇中的溶解度和体积传质系数

基于等体积饱和法搭建了气体在液体中溶解度与体积传质系数的实验测量系统,该实验系统温度、压力、溶解度、体积传质系数的扩展不确定度分别为0.02 K、0.01%、2%、4%。利用该实验系统测量了温度为323～343 K、压力为0.9～5.0 MPa范围内CO₂在正戊醇中的溶解度和体积传质系数。CO₂在正戊醇中的摩尔分数随着压力的升高而升高,在温度为323 K时,压力从2.5 MPa升高到3.2 MPa,溶解度升高26%。CO₂在正戊醇中的摩尔分数随着温度的升高而减小,在压力为0.9 MPa时,温度从323 K升高为343 K,溶解度降低26%。升高温度和压力都有利于提高体积传质系数,当温度和初始压力分别由323 K、1.1 MPa升高至343 K、5.0 MPa时,CO₂在正戊醇中的体积传质系数由0.0089 s^-1升高至 0.0175 s^-1。     

水力喷射-空气旋流器中微粒强化气液传质及其机理

在一种新型高效的气液传质设备--水力喷射-空气旋流器(WSA)中,研究了第三相固体粒子对气液传质的影响。分别采用化学吸收法(CO₂-空气-NaOH体系)和物理吸收法(CO₂-空气-H₂O体系)测定了不同固含率c_s、进口气速u_g、液体喷射速度u_L下的有效相界面积a和液膜传质系数k_L,并由此得到总体积传质系数k_La和增强因子E。结果表明,随着粒子固含率增大,k_L、a、k_La和E先增大后减小,存在一适宜固含率。在不同进口气速和液体喷射速度下,加入微粒后,k_L、a、k_La均增大,但E随进口气速和液体喷射速度增加而减小。微粒加入后,主要从a、k_L和表面更新频率S这3方面强化了气液传质,但主要是通过增强表面更新频率S而实现的。     

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。     

KINETICS OF SUPERCRITICAL FLUID EXTRACTION OF ETHANOL FROM AQUEOUS SOLUTION

A 1.3 dm³ high-pressure vessel was used to extract ethanol from aqueous solution of 10 wt% using supercritical carbon dioxide as a solvent. Experiments were carried out in a semibatch mode. A mathematical model based on the two-film theory was derived for estimating the over all mass transfer coefficient. The effects of operating variables, including pressure, CO₂ superficial velocity, and agitation rate, on the mass transfer coefficient were investigated. In general, the mass transfer coefficient increased with increasing pressure, CO₂ superficial velocity, and agitation rate. The concentration of ethanol recovered in the collector after 180 minutes reached 50 wt%, starting with a feed of 10 wt% ethanol.