流体动力学过程在流动腐蚀行为中的作用机制

在流动体系中,流场作用对腐蚀行为中的力学、离子传质以及界面反应等过程有着复杂的耦合影响,不同金属材料、不同溶液环境下流体流动发挥的作用也复杂多变,这些因素加剧了流动环境下的腐蚀机理研究的困难性。本文综述了流动腐蚀的研究现状,包括流动对腐蚀过程的影响机制、流动腐蚀研究的实验装置以及流动腐蚀中的关键影响因素,着重分析了流动通过改变腐蚀反应物/产物的质量传输速率对腐蚀反应动力学的影响机制,以及流动的剪切力作用对壁面产物膜的形成/破坏动力学过程的影响。提出了流动腐蚀在腐蚀界面演化与流场的交互作用、时空尺度跨度、流场-离子传质-界面反应的多场耦合联系以及不同流体力学参数匹配性等方面有待解决的问题,展望了流动腐蚀的发展方向。     

苏里格气田站厂管道腐蚀预测及对策研究

开展了苏里格气田站厂多相流模型研究，分别采用OLGA和Fluent软件对长庆油田苏里格气田某集气站和天然气处理厂易失效的典型管线，开展了气液两相流流态研究，揭示了不同运行条件下的气液两相流流态、流型及其转变规律，开展了CO₂腐蚀和冲刷腐蚀速率模拟计算，进行了多相流管道流流型综合腐蚀速率预测，并开展了管道内腐蚀失效风险评估，明确了管道失效高风险点。基于管道腐蚀速率预测结果和管道失效高风险点分析，提出了有效预防管道失效的技术对策。     

微通道内CO2吸收与传质及资源化利用的研究进展

由于在流体流动、传质、传热及反应等方面良好的调控能力,微化工技术成为化工学科重要的发展领域。综述了近年来以CO₂应用为背景的微化工系统中的多相流与传质的研究进展。从流体流动和传质机理出发,分别介绍了物理吸收和化学吸收过程的传质规律。总结了二氧化碳资源化利用的应用进展。展望了微化工技术在二氧化碳吸收与传质方面的发展前景。     

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。     

水溶液中电化学还原CO2的研究进展

CO₂作为一种潜在的碳资源,寻找一种有效的方法转移利用CO₂一直是社会关注的焦点。水溶液中电化学方法转化固定CO₂可在室温和常压下进行,通过选择不同电极和电极电势来改变产物、调控反应速率和选择性,因而具有潜在的优势。本文综述了水溶液中电化学还原CO₂的发展现状,介绍了水溶液中电还原CO₂的基本原理和电极上发生的主要反应;总结了水溶液中金属电极、气体扩散电极(GDEs)和复合电极等不同电极材料对CO₂还原产物的种类、选择性以及电流效率的影响;讨论了温度、CO₂分压等还原反应条件对反应速率和电流效率的影响。展望了水溶液中电还原CO₂技术的发展前景,认为利用水基溶液中丰富的[H],增强CO₂还原产物的燃料化程度,将在环境保护、资源利用和经济效益方面具有极大价值,符合绿色化学发展理念。     

高温环境下模拟CO2驱采出液中304不锈钢的腐蚀行为

现阶段随着CO₂驱油技术的普遍使用,采出液中CO₂的含量不断上升,使得采出系统中金属管道的腐蚀程度逐渐增大。为了掌握304不锈钢在高温环境下CO₂驱采出液中的腐蚀行为,室内配制了模拟CO₂驱采出液,测试了304不锈钢在高温环境下不同含量CO₂、不同腐蚀时间下的金属腐蚀速率,并对不同腐蚀时间下金属表面的微观形貌和腐蚀产物组成进行了表征。结果表明,随着CO₂含量和腐蚀时间的不断上升,金属的腐蚀速率上升;随着腐蚀时间的上升,金属表面的腐蚀产物逐渐增加,发生了局部区域析氢腐蚀过程;腐蚀产物膜主要由Fe₂O₃、Cr₂O₃和Fe CO₃组成。     

二氧化碳电化学还原反应器的研究进展

电化学还原二氧化碳（CO₂）可实现CO₂的资源化转化，是实现自然界“碳循环”、缓解因CO₂过度排放所引起诸多环境问题的关键技术。本文综述了CO₂电还原反应器的研究发展现状，并依据电解质的不同对比分析了各反应器的结构、传质特征及与之匹配阴极的CO₂转化活性与选择性。研究指出膜电极构型反应器是当前CO₂电还原反应器发展的主要方向，其电解质材料的优选不仅决定于其离子选择性与电导率，还需考虑电催化材料的性质与膜电极效率。最后，提出膜电极构型反应器内的过程强化技术与自支撑结构的阴极设计将成为CO₂还原研究发展的新方向。     

气液相变换热过程中界面腐蚀的基础研究进展

由于两相之间会不断转换,相变换热被称为复杂的传热传质过程,其过程中会引起相变腐蚀,如冷凝液滴腐蚀、气泡腐蚀以及多相流流动腐蚀等。目前对于气液相变腐蚀的研究集中在对腐蚀产物的表征、分析,忽略了相变过程中由于能量传递引起的界面变化对腐蚀的影响。本文从相变腐蚀机理、腐蚀防护两方面出发,系统地总结管道内外冷凝液滴腐蚀、气泡腐蚀与多相流流动腐蚀等气液相变腐蚀领域的研究进展,并对其中存在的问题进行总结,同时归纳了用于研究相变腐蚀过程的腐蚀预测模型,分析其应用场合以及各种模型的优势与不足,以期为研究气液相变腐蚀监测与控制的学者提供参考,并指出气液相变换热过程中的气液两相界面腐蚀问题是未来相变腐蚀研究的重要方向。     

碳毡负载Sn气体扩散电极CO2电化学还原性能

针对CO₂电化学还原中气体扩散电极可强化CO₂的传质,基于碳毡制备了负载锡-石墨烯催化层的新型气体扩散电极,研究了CO₂反应条件、电极厚度、催化剂载量及反应电位对CO₂电化学还原性能的影响。实验结果表明：与溶解态CO₂反应条件相比,采用气相CO₂反应条件电化学还原性能更好;一定范围内增加电极厚度和催化剂载量可以增加气-液-固三相反应界面,提升CO₂电化学还原性能;随着电解电位负移,甲酸产量增加,电流效率先增大后减小;实验中使用厚度为5 mm、载量为5 mg·cm^-2的电极,在-1.8 V（vs Ag/AgCl）条件下进行电化学还原时,平均电流密度为（12.79±1.27） mA·cm^-2,甲酸电流效率达到最佳为41.55%±2.50%。     

长庆油田原油输送管道内腐蚀预测分析

各种管道中水垢腐蚀产物碳酸盐和其他杂质沉积,会对管道形成强腐蚀.为了更好地解决管道内腐蚀问题,运用软件探讨温度、压力、管道直径、二氧化碳分压、管道倾斜角等参数对管道腐蚀速率的影响.结果表明:随着管道直径的增大,管道内的腐蚀程度降低;CO2气体分压的持续增加,对输送管道的腐蚀程度也会不断加重;同层流管道相比,拥塞段管道的腐蚀速率更高.基于以上条件下,对多相流管道相关的腐蚀问题做出详细分析,并且采用腐蚀风险分析方法预测管道可能发生腐蚀的位置.     

EFFECT OF ACETIC ACID ON CO2 CORROSION OF CARBON STEEL IN VAPOR-WATER TWO-PHASE HORIZONTAL FLOW

The effect of acetic acid on the corrosion behavior of X 65 and C 1018 carbon steel in vapor-water two-phase stratified flow (Vsg: 2 m/s; Vsl: 0.1 m/s) at 2 bars total pressure, 1.54 bars CO₂ partial pressure, pH 5.5, and 80°C was studied in a low pressure-high temperature multiphase flow horizontal loop using electrochemical and mass loss techniques. The liquid phase is composed of 1% NaCl aqueous solution containing different concentrations of acetic acid (500 to 5000 ppm total acetic acid), and the gas phase is composed of CO₂-acetic acid-water vapor mixture. The corrosion rates, on both the top and bottom of the line, increase with increase in acetic acid concentration, which was attributed to the contribution of hydrogen ions by the free acetic acid to the cathodic reaction. Partial coverage of the metal surface by FeCO₃ on both the top and bottom of the line is reported to be responsible for the observed localized corrosion. Surface analysis investigated with SEM and XRD is reported.

A vapor-liquid equilibrium model was developed for the system studied.     

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     

封存CO2裹挟可挥发性污染物的迁移模型分析

为了研究封存CO₂注入过程可挥发性污染物的释放和迁移特性,本文建立了CO₂-水-残余油多相流驱替过程中的污染物迁移模型。采用数学模拟方法分析了多相驱替过程和污染物迁移过程,并研究了相间传质特性、初始油相分布和CO₂注入速率等对污染物迁移过程的影响。研究表明:CO₂驱替过程将促使可挥发污染物进入CO₂相并随之在地层中迁移,逐渐形成相间传质区域。相间传质区域的演化反映了污染物释放和CO₂裹挟污染物迁移的特性。可挥发污染物的传质系数越大,相间传质区域越窄,油相饱和度衰减越快;油相初始饱和度较大时,其饱和度衰减相对缓慢,对应的相间传质区域也较窄。当CO₂注入速率增大时,相间传质区域增大,油相饱和度衰减变快。本文模型可用于不同地质储层环境下封存CO₂时可挥发性污染物的迁移特性分析,并用于封存CO₂的风险分析与评价。     

基于微吸收器的CO2吸收过程研究进展

微化工技术在流体流动、过程强化、传质与反应过程等领域备受关注,本文归纳整理了3种不同类型的微吸收器（微降膜吸收器、微通道吸收器和微网格吸收器）捕集CO₂过程中的水力学性质和传质过程及其机理研究进展,并对3种微吸收器吸收CO₂过程中存在的问题进行分析总结,同时对微吸收器能快速工业化提出展望。其中重点介绍了微通道泰勒流吸收器的水力学流动特性,包括泰勒流气泡的生成机制、气泡和液弹的长度、气泡的输运和运动速度、气泡截面形状及液膜厚度和气液两相流压降;归纳了微通道泰勒流吸收过程的传质过程机理和传质系数的模型以及不同影响因素（通道截面尺寸,通道长度,主通道结构及入口形状,气、液相组成及其流速,吸收剂和系统压力）作用下CO₂吸收效率和传质系数的研究进展。     

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.     

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.     

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。     

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.     

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。