水吸收CO_2过程界面对流的激光诱导荧光观测

建立了采用激光诱导荧光技术观测水吸收CO_2过程中界面对流现象的实验装置,利用荧光素钠作为荧光剂,通过标定获得了CO_2在水中溶解浓度与荧光强度的关系,进而获得了定量测量水中CO_2浓度分布的实验方法。通过建立的实验装置和方法,测量了水吸收CO_2过程中液体近界面Rayleigh对流发生时的浓度分布演化过程。利用实验结果对文献中报道的临界Rayleigh数进行了验证;并对上述吸收体系的界面传质由分子扩散主导逐步转变为对流传质主导的过程,以及Rayleigh对流对吸收过程界面传质的强化进行了定量分析。     

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。     

Rayleigh对流及其对界面传质影响模拟的格子Boltzmann方法

针对乙醇吸收CO₂过程中,由CO₂通过界面向液体乙醇传递所导致的Rayleigh对流现象的模拟,建立了二维格子Boltzmann方法（LBM）。采用浓度分布函数和流体质点密度函数的双分布模型格子Boltzmann方法,同时引入由浓度差导致的重度差作为外加力,实现了流体中浓度场与速度场的模拟。应用所建立的LBM方法,对界面具有多个离散CO₂扩散源的二维区域液相Rayleigh对流现象进行了模拟,结果显示,模拟得到的浓度分布结构与文献中实验结果相一致。通过考察Rayleigh对流和浓度分布结构,分析了Rayleigh对流存在条件下的传递规律。通过采用LBM方法对浓度场模拟可以定量给出液相界面瞬时传质通量。计算结果表明,瞬时传质通量随时间的增长先增加后减小,这种变化与相似文献   

界面传质中Rayleigh对流的定量分析

通过纹影光路观察了特定气液传质装置中乙醇吸收CO₂过程所引发的Rayleigh对流在垂直界面方向上的发展过程。随着溶质吸收的进行,液层的流体稳定性变弱,扰动加剧气液界面失稳并发生湍动,进而发展为羽状流并逐步向液相主体发展,在此过程中伴随着对流胞的融合与增长。液层的浓度分布可通过对相应液层纹影图像进行定量分析获得。液层浓度分布和瞬时传质系数变化表征了Rayleigh对流的引发与发展及其对传质过程的强化效果,界面浓度分布及临界Rayleigh数解释了非均匀传质对湍动的引发机理。羽状流将高浓度液体快速带入主体,加速了近界面液层与主体液层的混合,增强了气液传质。     

气相第2组分对水溶解CO2过程界面对流影响的LIF观测

采用激光诱导荧光（LIF）观测方法考察了在气相中分别添加乙醇和二氯甲烷分别对CO₂在水中溶解过程界面对流的影响,得到了液相中CO₂浓度分布及其演化的观测结果,通过物料衡算得到了相应条件下的液相传质系数。CO₂溶解过程会出现由密度梯度引起的Rayleigh对流。实验结果表明,当添加的乙醇含量小于8.47 mg·L^-1时,Rayleigh对流会被增强,进而促进了CO₂的溶解;随着气相中乙醇含量的增大,Rayleigh对流反而被抑制;气相添加二氯甲烷会显著增强Rayleigh对流,提高了CO₂的传质速率,随着气相二氯甲烷含量的增大,CO₂在水中溶解过程的液相传质系数呈现先加强后恒定的趋势。     

水溶解CO2过程界面对流现象的PIV/LIF测量及传质系数预测

建立了用于观测水溶解CO₂过程界面Rayleigh对流现象的粒子成像测速（PIV）和激光诱导荧光（LIF）技术联用方法,同时获得了该对流传质过程的液相速度场及浓度分布,定量观测了Rayleigh对流的发展过程。经界面对流发生条件下传质过程的分析,指出Rayleigh对流过程的涡量是影响传质过程的主要因素,给出了传质系数随涡量的变化关系和相应的关联式,进而为通过液相速度场的测量预测Rayleigh对流条件下的液相传质系数提供了一种有效的方法。     

吸收过程Rayleigh对流非稳态数值模拟

通过应用有限元方法,对气液吸收过程中出现的Rayleigh对流发生过程进行了数值模拟计算,得到了液相Rayleigh对流发生时的流场分布和浓度分布定量信息;利用激光纹影仪光学方法,获得了乙醇吸收CO2过程中Rayleigh对流的纹影图像,通过比较模拟计算结果和实验纹影图像,证实模拟计算结果的正确;在模拟计算和实验结果的基础上,对传质过程中Rayleigh对流对传质过程的影响进行了定性和定量的分析,揭示了界面传质导致的Rayleigh对流产生发展过程及对传质的影响.     

受限空间内浮升气泡与液体间传质行为实验研究

采用紫外诱导荧光(UIF)实验方法,研究Hele-Shaw狭缝受限尺度对受限空间内浮升气泡流体力学与气液传质行为的影响。实验中以二苯并[b,e]吡啶作为荧光剂实现了受限空间内CO₂溶液浓度分布及其气泡运动速度的定量测量,获得了CO₂在受限空间内运动过程中的传质量和气泡动力学参数,并分别计算气泡受限空间内液膜区和自由接触区的传质速率。分析得到受限空间中不同狭缝宽度内CO₂的传质行为,分析了受限尺度对CO₂-水体系传质过程的影响。     

受限空间内浮升气泡与液体间传质行为实验研究

采用紫外诱导荧光(UIF)实验方法,研究Hele-Shaw狭缝受限尺度对受限空间内浮升气泡流体力学与气液传质行为的影响。实验中以二苯并[b,e]吡啶作为荧光剂实现了受限空间内CO₂溶液浓度分布及其气泡运动速度的定量测量,获得了CO₂在受限空间内运动过程中的传质量和气泡动力学参数,并分别计算气泡受限空间内液膜区和自由接触区的传质速率。分析得到受限空间中不同狭缝宽度内CO₂的传质行为,分析了受限尺度对CO₂-水体系传质过程的影响。     

界面传质中Rayleigh对流的定量分析

通过纹影光路观察了特定气液传质装置中乙醇吸收CO2过程所引发的Rayleigh对流在垂直界面方向上的发展过程。随着溶质吸收的进行,液层的流体稳定性变弱,扰动加剧气液界面失稳并发生湍动,进而发展为羽状流并逐步向液相主体发展,在此过程中伴随着对流胞的融合与增长。液层的浓度分布可通过对相应液层纹影图像进行定量分析获得。液层浓度分布和瞬时传质系数变化表征了Rayleigh对流的引发与发展及其对传质过程的强化效果,界面浓度分布及临界Rayleigh数解释了非均匀传质对湍动的引发机理。羽状流将高浓度液体快速带入主体,加速了近界面液层与主体液层的混合,增强了气液传质。     

伴有Rayleigh对流的气液传质理论

浓度梯度导致的Rayleigh对流会对界面传质产生重要影响。采用格子Boltzmann方法(LBM)对吸收过程伴有Rayleigh对流的气液传质理论进行了分析。针对表面更新理论,提出了将近界面处羽状对流结构的宽度作为特征尺度来求得表面更新时间。结果表明,Rayleigh对流的发生能够有效减小双膜理论中的液膜厚度;液相传质系数的LBM模拟值与表面更新理论预测值吻合较好。     

Investigation of mass transfer model of CO2 absorption with Rayleigh convection using multi-relaxation time lattice Boltzmann method

CO₂ absorption into absorbents is a widely used method to reduce carbon emissions, in which the concentration gradient near the gas-liquid interface may induce Rayleigh convection (RC). Once RC occurs, the mass transfer rate will be significantly enhanced. Therefore, it is necessary to explore the mass transfer enhancement mechanism further and develop a penetration/surface divergence hybrid mass transfer model. In this study, we conduct research on the process of CO₂ absorption into ethanol with RC. Firstly, we use a multi-relaxation time lattice Boltzmann method to simulate the absorption process and obtain the flow and concentration fields. And we also verify the reliability of the numerical simulation results by comparing with the experimental results. Then, we analyze the characteristics of non-uniform flow and concentration fields in RC. Moreover, we divide the near-interface region into diffusion-dominated and convection-dominated mass transfer zones by checking whether the horizontal average velocity is greater than 1.0×10^-4 m·s^-1. Furthermore, based on the differences in mass transfer mechanisms of the aforementioned two zones, we propose a penetration/surface divergence hybrid model to predict the instantaneous mass transfer coefficient. The prediction results demonstrate that the hybrid model can precisely predict the instantaneous mass transfer coefficient of the entire CO₂ absorption process. Our proposed hybrid model provides a promising way to deal with the complex mass transfer problems with non-uniform flow and concentration fields.     

Entransy dissipation analysis of interfacial convection enhancing gas–liquid mass transfer process based on field synergy principle

An exploration of the gas CO2 absorbed into liquid ethanol accompanied with Rayleigh convection is performed by analyzing the mass entransy dissipation; this new statistical quantity is introduced to describe the irreversibility of mass transfer potential capacity. Based on the general advection–diffusion differential equation for an unsteady mass transfer process, the variation of the included angle between the velocity vector and concentration gradient fields is investigated to reveal the underlying mechanism of interfacial convection enhancing mass transfer. Results show some identical characteristics with the qualitative analyses of the synergy effects generated by the concentration and velocity fields after interfacial convection occurring for a boundary condition of fixed surface concentration. And the equivalent mass resistance for convective mass transfer process presents the similar variation with the reciprocal of instantaneous mass transfer coefficient. Accordingly, it is reasonable to be seen that mass transfer dissipation rate could be provided to assess the convection strength and explain fundamentally how Rayleigh convection improves mass transfer performance through establishing a close relationship between the mass transfer capacity and field synergy principle from the view of mass transfer theory.     

3D multiphase flow simulation of Marangoni convection on reactive absorption of CO2 by monoethanolamine in microchannel

A multiphase flow 3D numerical simulation method employing the coupled volume of fluid (VOF) and level set model is established to study the reactive absorption of CO₂ by the monoethanolamine (MEA) aqueous solution in a falling film microchannel. Based on the flow-reaction-mass transfer model of the MEA-CO₂ system in the falling film microchannel, the enhancement effect of the Marangoni convection in this reactive absorption process is analyzed. The enhancement factor of the Marangoni convection obtained in this work is in good agreement with experimental results in the literature. With consideration of the absorption ratio as well as the enhancement effect of the Marangoni convection, the influence of different MEA concentrations on absorption of CO₂ is investigated. Furthermore, the appropriate MEA concentration for absorption enhanced by the Marangoni convection is acquired.     

Pore-scale study based on lattice Boltzmann method of density driven natural convection during CO2 injection project

Saline aquifers are chosen for geological storage of greenhouse gas CO₂ because of their storage potential. In almost all cases of practical interest, CO₂ is present on top of the liquid and CO₂ dissolution leads to a small increase in the density of the aqueous phase. This situation results in the creation of negative buoyancy force for downward density-driven natural convection and consequently enhances CO₂ sequestration. In order to study CO₂ injection at pore-level, an isothermal Lattice Boltzmann Model (LBM)with two distribution functions is adopted to simulate density-driven natural convection in porous media with irregular geometry obtained by image treatment. The present analysis showed that after the onset of natural convection instability, the brine with a high CO₂ concentration infringed into the underlying unaffected brine, in favor of the migration of CO₂ into the pore structure. With low Rayleigh numbers, the instantaneous mass flux and total dissolved CO₂ mass are very close to that derived from penetration theory (diffusion only), but the fluxes are significantly enhanced with high Ra number. The simulated results show that as the time increases, some chaotic and recirculation zones in the flow appear obviously, which promotes the renewal of interfacial liquid, and hence enhances dissolution of CO₂ into brine. This study is focused on the scale of a few pores, but shows implications in enhanced oil/gas recovery with CO₂ sequestration in aquifers.     

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。