Investigations on the ability of di‐isopropanol amine solution for removal of CO2 from natural gas in porous polymeric membranes

In this study, capture of CO₂ and H₂S from natural gas mixture using porous polymeric membranes has been investigated numerically to assess the capacity of a novel absorbent, di‐isopropanol amine (DIPA), in CO₂ removal. Diffusion of acid gases through porous polymeric membranes was simulated by employing CFD techniques and considering a gas feed stream, a porous membrane and a reaction medium. For solving conservation equations, finite element method was applied to calculate the rate of CO₂ and H₂S absorption in the membrane. The type of membrane in this work is a hollow‐fiber module. According to the modeling results, a high H₂S removal can be achieved by DIPA absorber. Moreover, CO₂ was captured from natural gas in an efficient manner in low gas/liquid flow rates. POLYM. ENG. SCI., 55:598–603, 2015. © 2014 Society of Plastics Engineers     

Investigation of hydrodynamic performance and effective mass transfer area for Sulzer DX structured packing

The hydrodynamic performance in terms of pressure drop (?P) and liquid holdup (h_L), and tshe effective mass transfer area (a_e) of Sulzer DX structured packing were investigated at 293.15 K and 101.3 kPa. In addition, the flooding velocity (u_F) was also calculated based on the experimental results of liquid holdup, and the effective voidage correction factor (?) was obtained by combining the Billet model and the experimental effective fraction. The liquid volume method and pressure difference from just below to above the column packing approach are used to describe the hydrodynamic performance in a structured packing column. Experimental results showed that the operational conditions in terms of gas flow rate, liquid flow rate, viscosity, and liquid systems strongly affect the hydrodynamic performance. The experimental comparison between the pressure drop profiles in air‐water (polyethylene oxide [PEO]) and MEA‐H₂O‐CO₂ systems indicated that both the reacting MEA and CO₂ partial pressure can enhance the pressure drop value. In addition, the Bain‐Haugen correlation model was developed to predict the flooding velocity data with an acceptable AARD of 8.1%, and a model was also successfully proposed to predict the values of liquid holdup with an AARD of 11.8%, which is lower than 14.7% in Billet model. Furthermore, the effective mass transfer area was found to be increased by increasing both the liquid and gas flow rate by using NaOH‐H₂O‐CO₂ system. A model was also proposed to calculate the experimental a_e with an acceptable AARD% of 19.52, and this built model (Eq. 39) can reasonably explain the experimental phenomenon. © 2018 American Institute of Chemical Engineers AIChE J, 64: 3625–3637, 2018     

Computational fluid dynamics simulation of reactive absorption of CO2 in a structured packed column

In this study, multiphase Eulerian computational fluid dynamics (CFD) modelling is developed to predict the hydrodynamics, mass transfer, and chemical absorption of CO₂ using a monoethanolamine (MEA) solution in a structured packed column. First, the hydrodynamic simulation of liquid dispersion in a structured packed bed using a two-dimensional CFD is performed. The simulation results of the radial distribution of the liquid holdup are compared with the literature experimental data. The model prediction matches the experimental data at the top position of the column, whereas a slight deviation is found at the bottom position of the column. Using a validated CFD model, the reactive mass transfer is modelled to study CO₂ capture in a structured packed column with Mellapak 500.X. The model results are compared to the literature experimental results of CO₂ mole fractions along the height of the column. It is found that the model results match the experimental findings. Furthermore, CFD modelling is extended to investigate the influence of operating conditions such as gas and liquid velocities on CO₂ removal efficiency. The present CFD model demonstrates the porous media approach for reactive absorption of CO₂ in a structural packed bed.     

Reduction of amine mist emissions from a pilot-scale CO2 capture process using charged colloidal gas aphrons

In the CO₂ capture process from coal-derived flue gas where amine solvents are used, the flue gas can entrain small liquid droplets into the gas stream leading to emission of the amine solvent. The entrained drops, or mist, will lead to high solvent losses and cause decreased CO₂ capture performance. In order to reduce the emissions of the fine amine droplets from CO₂ absorber, a novel method using charged colloidal gas aphron (CGA) generated by an anionic surfactant was developed. The CGA absorption process for MEA emission reduction was optimized by investigating the surfactant concentration, stirring speed of the CGA generator, and capture temperature. The results show a significant reduction of MEA emissions of over 50% in the flue gas stream exiting the absorber column of a pilot scale CO₂ capture unit.     

Separation of greenhouse gases from gas mixtures using nanoporous polymeric membranes

Removal of greenhouse gases from gas streams using porous membranes was carried out in this work. Theoretical studies were performed in terms of mathematical modeling and numerical simulation of CO₂ capture in a flat‐sheet membrane contactor. Numerical simulation was performed using computational fluid dynamics (CFD) of mass and momentum transfer in the membrane module for laminar flow conditions. Physical absorption was considered in the simulations for absorption of CO₂ in pure water. CO₂ concentration distribution in the membrane module was determined through numerical solution of continuity equation coupled with the Navier‐Stokes equations. The modeling predictions indicated that the CO₂ concentration difference is not appreciable in the membrane direction. Moreover, velocity distribution was determined in the liquid side of membrane contactor. CFD also represents a design and optimization tool for membrane gas separation processes. POLYM. ENG. SCI., 55:975–980, 2015. © 2014 Society of Plastics Engineers     

Mass transfer performance and correlations for CO2 absorption into aqueous blended of DEEA/MEA in a random packed column

The mass transfer performance of CO₂ absorption into blended N,N‐diethylethanolamine (DEEA)/ethanolamine (MEA) solutions was investigated using a lab‐scale absorber (H = 1.28 m, D = 28 mm) packed with Dixon ring random packing. The mass transfer coefficient K_Ga_v, the unit volume absorption rate Φ, outlet concentration of CO₂ (y_CO2), and the bottom temperature T_bot of CO₂ in aqueous DEEA/MEA solutions were determined over the feed temperature range of 298.15–323.15 K, lean CO₂ loading of 0.15–0.31 mol/mol, over a wide range of liquid flow rate of 3.90–9.75 m³/m²‐h, by using inert gas flow rate of 26.11–39.17 kmol/m²‐h and 6–18 kPa CO₂ partial pressure. The results show that liquid feed temperature, lean CO₂ loading, liquid flow rate, and CO₂ partial pressure had significant effect on those parameters. However, the inert gas flow rate had little effect. To allow the mass transfer data to be really utilized, K_Ga_v and y_out correlations for the prediction of mass transfer performance were proposed and discussed. © 2017 American Institute of Chemical Engineers AIChE J, 63: 3048–3057, 2017     

Gas−liquid multiphase computational fluid dynamics (CFD) of amine absorption column with structured-packing for CO2 capture

The gas−liquid multiphase Eulerian computational fluid dynamics (CFD) model was used to investigate hydrodynamics and CO₂ removal efficiency of a pilot-scale amine absorber with structured-packing. The structured-packing was represented by a porous media zone having porous resistance, gas−liquid interfacial drag force, and liquid dispersion force. This study aimed to find a reasonable way to identify four modification factors of the Ergun coefficient that determine the hydrodynamic characteristics of structured-packing. The two modification factors (a and b) for porous resistance were mainly related to the liquid holdup (h_L) with respect to the liquid load. The other two factors (c and d) for gas−liquid interfacial drag force depended on the specific wet pressure drop (ΔP_wet/L) versus the gas load factor. The h_L and ΔP_wet/L increased in parallel with the increase of a and c, respectively, while the slopes of h_L and ΔP_wet/L increased with b and d, respectively.     

A new design concept of structured packing column auxiliaries

This paper discusses the criteria for obtaining an improved performance of structured packing columns in gas-liquid contacting, by improving the liquid and gas distributors. A new liquid distributor design, specific for structured packing columns is presented. Experimental measurements which quantify the improvements attained by the new distributor are also presented. Furthermore, gas flow distribution requirements for structured packing columns are discussed. Three “case studies” indicative of the implementation of the proposed distributor concept in industrial columns are included. Case (a) CO₂/MEA removal column, case (b) ammonia splitter and case (c) acid gas neutralization column.     

规整填料塔内气-液两相并流流动的CFD研究

应用FLUENT,即一款流体力学计算软件,对规整填料塔内的气液两相并流流动时的液相分布进行了研究,用数学方法拟合出压降和持液量之间的定量关系,并通过实验进行了验证。基于Mellapak350Y填料建立了物理模型,采用的方程是RNG k-ε湍流模型封闭动量方程。模拟过程中引入了表面张力源项以及相间作用力源项。模拟结果和实验结果吻合良好,表明了求解规整填料塔内两相并流流动的方法是合理的。     

Carbon dioxide absorption in a cross-flow rotating packed bed

This work investigates the feasibility of applying the cross-flow rotating packed bed (RPB) to the removal of carbon dioxide (CO₂) by absorption from gaseous streams. Monoethanolamine (MEA) aqueous solution was used as the model absorbent. Also, other absorbents such as the NaOH and 2-amino-2-methyl-1-propanol (AMP) aqueous solutions were compared with the MEA aqueous solution. The CO₂ removal efficiency was observed as functions of rotor speed, gas flow rate, liquid flow rate, MEA concentration, and CO₂ concentration. Experimental results indicated that the rotor speed positively affects the CO₂ removal efficiency. Our results further demonstrated that the CO₂ removal efficiency increased with the liquid flow rate and the MEA concentration; however, decreased with the gas flow rate and the CO₂ concentration. Additionally, the CO₂ removal efficiency for the MEA aqueous solution was superior to that for the NaOH and AMP aqueous solutions. Based on the performance comparison with the conventional packed bed and the countercurrent-flow RPB, the cross-flow RPB is an effective absorber for CO₂ absorption process.     

Post-combustion CO2 capture process: Equilibrium stage mathematical model of the chemical absorption of CO2 into monoethanolamine (MEA) aqueous solution

This paper deals with the modeling and optimization of the chemical absorption process to CO₂ removal using monoethanolamine (MEA) aqueous solution. Precisely, an optimization mathematical model is proposed to determine the best operating conditions of the CO₂ post-combustion process in order to maximize the CO₂ removal efficiency. Certainly, the following two objective functions are considered for maximization: (a) ratio between the total absorbed CO₂ and the total heating and cooling utilities and (b) ratio between total absorbed CO₂ and the total amine flow-rate.Temperature, composition and flow-rate profiles of the aqueous solution and gas streams along the absorber and regenerator as well as the reboiler and condenser duties are considered as optimization variables. The number of trays or height equivalent to a theoretical plate (HETP) on the absorber and regenerator columns as well as the CO₂ composition in flue gas are treated as model parameters. Correlations used to compute physical-chemical properties of the aqueous amine solution are taken from different specialized literature and are valid for a wide range of operating conditions. For the modeling, both columns (absorber and regenerator) are divided into a number of segments assuming that liquid and gas phases are well mixed.GAMS (General Algebraic Modeling System) and CONOPT are used, respectively, to implement and to solve the resulting mathematical model.The robustness and computational performance of the proposed model and a detailed discussion of the optimization results will be presented through different case studies. Finally, the proposed model cannot only be used as optimizer but also as a simulator by fixing the degree of freedom of the equation system.     

Comprehensive modeling and CFD simulation of absorption of CO2 and H2S by MEA solution in hollow fiber membrane reactors

A comprehensive mathematical model has been developed for the simulation of simultaneous chemical absorption of carbon dioxide and hydrogen sulfide by means of Monoethanolamine (MEA) aqueous solution in hollow fiber membrane reactors is described. In this regard, a perfect model considering the entrance regions of momentum, energy, and mass transfers was developed. Computational Fluid Dynamics (CFD) techniques were applied to solve governing equations, and the model predictions were validated against experimental data reported in the literature and excellent agreement was found. Effects of different disturbances on the dynamic behavior of the reactor were investigated. Moreover, effects of various parameters such as wetting fraction, gas and liquid inlet velocities, inlet temperature of the solvent, MEA concentration, and CO₂ and H₂S compositions were carefully studied. It was found that for large values of gas velocity or small values of liquid velocity, the thermal energy equation can play an important role in the model predictions. © 2013 American Institute of Chemical Engineers AIChE J 60: 657–672, 2014     

Pilot plant study of post-combustion carbon dioxide capture by reactive absorption: Methodology, comparison of different structured packings, and comprehensive results for monoethanolamine

Post-combustion carbon capture (PCC) from fossil fuel power plants by reactive absorption can substantially contribute to reduce emissions of the greenhouse gas CO₂. To test new solvents for this purpose small pilot plants are used. The present paper describes results of comprehensive studies of the standard PCC solvent MEA (0.3 g/g monoethanolamine in water) in a pilot plant in which the closed cycle of absorption/desorption process is continuously operated (column diameters: 0.125 m, absorber/desorber packing height: 4.25/2.55 m, packing type: Sulzer BX 500, flue gas flow: 30-110 kg/h, CO₂ partial pressure: 35-135 mbar). The data establish a base line for comparisons with new solvents tested in the pilot plant and can be used for a validation of models of the PCC process with MEA. The ratio of the solvent to the flue gas mass flow is systematically varied at constant CO₂ removal rate, and CO₂ partial pressure in the flue gas. Optimal operating points are determined. In the present study the structured packing Sulzer BX 500 is used. The experiments with the removal rate variation are carried out so that the results can directly be compared to those from a previous study in the same plant that was carried out using Sulzer Mellapak 250.Y. A strategy for identifying the influence of absorption kinetics on the results is proposed, which is based on a variation of the gas load at a constant L/G ratio and provides valuable insight on the transferability of pilot plant results.     

Gas holdup and energy dissipation in liquid‐gas ejectors

BACKGROUND: Ejectors have excellent mass transfer characteristics with energy efficiency and can be used in place of conventional countercurrent systems, namely, packed bed contactors as well as venturi scrubbers, cyclones and airlift pumps. Although a number of papers have been published in the recent past, none of them provides a theoretical basis for the prediction of gas phase holdup. In this work an attempt has been made to develop a theoretical basis for predicting gas phase holdup based on first principles using Nguyen and Spedding's distribution function (C_o) and initial value parameter (B). RESULTS: In the present work, measurements and correlations are reported for the gas holdup and energy dissipation in a liquid‐gas ejector. The holdup data have been correlated using the theoretical models proposed by Nguyen and Spedding, 26 with an estimated initial value parameter B and the distribution function C_o. The throat and diffuser loss coefficients were found to be constant up to a gas/liquid flow ratio of 1.6 and then it was found to be a function of area ratio, physical properties and gas holdup. CONCLUSIONS: The present proposed correlations for gas phase holdup and energy dissipation, E_mix, should be useful for the efficient design of co‐current ejectors for gas‐liquid contacting, in particular for the removal of CO₂ from natural gas, since the viscosity and surface tension ranges covered in the present study are essentially those encountered in amine–carbon dioxide systems. Copyright © 2008 Society of Chemical Industry     

Pilot plant study of two new solvents for post combustion carbon dioxide capture by reactive absorption and comparison to monoethanolamine

Application of new solvents will substantially contribute to the reduction of the energy demand for the post combustion capture of CO₂ from power plant flue gases. The present work describes tests of such new solvents in a gas-fired pilot plant, which comprises the complete absorption/desorption process (column diameters 0.125 m, absorber/desorber packing height 4.25/2.55 m, packing type: Sulzer BX 500, flue gas flow 30–100 kg/h, CO₂ partial pressure 35–135 mbar). Two new solvents CESAR1 (0.28 g/g 2-amino-2-methyl-1-propanol+0.17 g/g piperazine+0.55 g/g H₂O) and CESAR2 (0.32 g/g 1, 2-ethanediamine+0.68 g/g H₂O), which were developed in an EU-project, were systematically studied and compared to MEA (0.3 g/g monoethanolamine+0.7 g/g H₂O). The two new solvents and MEA were studied in the same way in the pilot plant and detailed results are reported for all solvents. In the present study the structured packing Sulzer BX 500 is used. The measurements are carried out at a constant CO₂ removal rate of 90% by an adjustment of the regeneration energy in the desorber for systematically varied solvent flow rates. An optimal solvent flow rate leading to a minimum energy requirement is found from these studies. Direct comparisons of such results can be misleading if there are differences in the kinetics of the different solvent systems. The influence of kinetic effects is experimentally studied by varying the flue gas flow rate at a constant ratio of solvent mass flow to flue gas mass flow and constant CO₂ removal rate. Results from these studies indicate similar kinetics for CESAR1, CESAR2 and MEA. The direct comparison of the pilot plant results for these solvents is therefore justified. Both CESAR1 and CESAR2 show improvements compared to MEA. The most promising is CESAR1 with a reduction of about 20% in the regeneration energy and 45% in the solvent flow rate.     

单乙醇胺吸收CO2的热力学模型和过程模拟

采用非随机双流体电解质（ENRTL）热力学模型,通过拟合单乙醇胺（MEA）的饱和蒸气压、热容数据,MEA和水（H₂O）二元体系的汽液平衡、热容、混合热数据,以及二氧化碳（CO₂）在MEA水溶液中的溶解度数据,建立了MEA吸收CO₂的热力学模型,并用核磁共振（NMR）组成数据成功地进行了验证。在此模型基础上,利用平衡级模型建立了MEA吸收/解吸CO₂的过程模拟,利用文献中中试工厂数据验证了过程模拟的准确性。对于质量分数为30%的MEA溶液,固定吸收塔CO₂去除率为90%的条件下,当吸收塔液气质量流率比值为2时,再沸器能耗最小,为3.64 GJ·（t CO₂）^-1。     

The influence of random packed column parameters on the liquid holdup and interfacial area

Carbon dioxide capture via solvent absorption in packed columns has emerged as a potential technology to mitigate coal-fired power plant CO₂ emissions. Parameters, including packing types, solvent properties, and operating conditions, could potentially affect the packed column CO₂ capture efficiency. To understand the importance of those parameters and help packed column optimization, a design of experiments (DoEs) method was proposed to generate input parameter matrix. Combined with multiphase computational fluid dynamics (CFD), the random packed column parameter influence on the liquid holdup and interfacial area can be efficiently investigated. Surrogate-based sensitivity analysis shows that the solvent flow rate and contact angle are key factors dictating liquid holdup and interfacial area. On the other hand, solvent viscosity has a marginal impact on the interfacial area. The sensitivity scores were calculated for each input parameter to guide the selection of dimensionless numbers for the liquid holdup and interfacial area correlation development.     

Holdup and Pressure Drop of Packed Beds Containing a Modular Catalytic Structured Packing

A comparative experimental study has been carried out to establish the hydraulic behavior of a new modular catalytic packing (Sulzer's Katapak^®‐SP 12) and the hybrid packed bed consisting of a catalytic packing section placed in between two sections comprising elements of a high capacity structured packing (MellapakPlus 752.Y). Air‐water experiments were carried out at ambient conditions using a Perspex column with an internal diameter of 0.45 m. As expected, the liquid holdup and the pressure drop of the combined bed were between those measured for beds consisting purely of the catalytic and structured packings. However, unlike the two reference beds, the combined bed exhibited a clear upper gas load limit due to a pronounced liquid buildup at the transition from the structured packing to the top element of the catalytic packing section. Also it appeared that the Delft model, with appropriate packing geometry modifications is capable of reliably predicting the preloading region holdup and pressure drop of a hybrid packed bed containing Katapak‐SP.     

Direct dual layer spinning of aminosilica/Torlon® hollow fiber sorbents with a lumen layer for CO2 separation by rapid temperature swing adsorption

The direct dual layer spinning of Torlon^®/silica hollow fibers with a neat Torlon^® lumen layer is reported here for the first time. The dual layer fibers containing a porous Torlon^®/silica main structure and a dense, pure Torlon^® polymer bore‐side coating provide a simplified, scalable platform from which to construct hollow fiber amine sorbents for postcombustion CO₂ capture. After fiber spinning, an amine infusion process is applied to incorporate PEI into the silica pores. After combining dilute Neoprene treatment followed by poly(aramid)/PDMS treatment, a helium permeance of the fiber sorbents of 2 GPU with a He/N₂ selectivity of 7.4 is achieved. Ten of the optimized amine‐containing hollow fibers are incorporated into a 22‐inch long, 1/2 inch OD shell‐and‐tube module and the module is then exposed on the shell side to simulated flue gas with an inert tracer (14 mol % CO₂, 72 mol % N₂, 14 mol % He [at 100% R.H.]) at 1 atm and 35°C in a RTSA system for preliminary CO₂ sorption experiments. The fibers are found to have a breakthrough and equilibrium CO₂ capacity of 0.8 and 1.2 mmol/g‐ dry fiber sorbent, respectively. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41845.     

CO2 Absorption into Aqueous Solutions of a Polyamine (PZEA), a Sterically Hindered Amine (AMP), and their Blends

Among numerous techniques existing for reducing CO₂ emissions, CO₂ capture by absorption in aqueous alkanolamine solutions was specifically studied in this work. For the choice of the adequate amine solution, two major criteria must be taken into account: absorption performances (higher with primary and secondary amines) and energy costs for solvent regeneration (more interesting with tertiary and sterically hindered amines). The different types of amines can also be mixed in order to combine the specific advantages of each type of amines, an activation phenomenon being observed. Aqueous solutions of (piperazinyl‐1)‐2‐ethylamine (PZEA, a polyamine known as absorption activator) and 1‐amino‐2‐propanol (AMP, a sterically hindered amine), pure or mixed with other amines, are experimentally compared with respect to CO₂ removal performances by means of absorption test runs achieved in a special gas‐liquid contactor at 25 °C. The positive impact of addition of PZEA to monoethanolamine (MEA), N‐methyldiethanolamine (MDEA), and AMP solutions was clearly highlighted. The absorption performances have also been satisfactorily simulated with coherent physicochemical data.