Dynamic modeling of CO2 absorption from coal-fired power plants into an aqueous monoethanolamine solution

Among carbon capture and storage (CCS), the post-combustion capture of carbon dioxide (CO₂) by means of chemical absorption is actually the most developed process. Steady state process simulation turned out as a powerful tool for the design of such CO₂ scrubbers. Besides steady state modeling, transient process simulations deliver valuable information on the dynamic behavior of the system. Dynamic interactions of the power plant with the CO₂ separation plant can be described by such models. Within this work a dynamic process simulation model of the absorption unit of a CO₂ separation plant was developed. For describing the chemical absorption of CO₂ into an aqueous monoethanolamine solution a rate based approach was used. All models were developed within the Aspen Custom Modeler^® simulation environment. Thermo physical properties as well as transport properties were taken from the electrolyte non-random-two-liquid model provided by the Aspen Properties^® database. Within this work two simulation cases are presented. In a first simulation the inlet temperature of the flue gas and the lean solvent into the absorber column was changed. The results were validated by using experimental data from the CO₂SEPPL test rig located at the Dürnrohr power station. In a second simulation the flue gas flow to the separation plant was increased. Due to the unavailability of experimental data a validation of the results from the second simulation could not be achieved.     

Generic AI models for mass transfer coefficient prediction in amine-based CO2 absorber,Part II: RBFNN and RF model

In this work, the radial basis function neural network (RBFNN) and random forest (RF) algorithms were employed to develop generic AI models predicting mass transfer coefficient in amine-based CO₂ absorber. The models with operating parameters as input gave quite different prediction performance in different CO₂ absorption systems. To secure better applicability, extra parameters related to amine type and packing characteristics were introduced to reasonably describe mass transfer behaviors, respectively. Moreover, the generic models were proposed by considering all influencing factors of mass transfer in CO₂ absorber column. Furthermore, the performance of BPNN, RBFNN, and RF models was completely compared and fully discussed in terms of AARE. All three generic models could predict mass transfer coefficient of CO₂ absorber very well. It was found that the BPNN models provide the best predication with AAREs of below 5%. The developed generic model could serve as a fast and efficient tool for preliminary selection and evaluation of potential amines for CO₂ absorption. The framework of generic ML model development was also clearly presented, which could provide theoretical basis and practical guidance for the implementation and application of ML models in the carbon capture field.     

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.     

Dynamic modelling of CO2 absorption for post combustion capture in coal-fired power plants

Power generation from fossil fuel-fired power plants is the largest single source of CO₂ emissions. Post combustion capture via chemical absorption is viewed as the most mature CO₂ capture technique. This paper presents a study of the post combustion CO₂ capture with monoethanolamine (MEA) based on dynamic modelling of the process. The aims of the project were to compare two different approaches (the equilibrium-based approach versus the rate-based approach) in modelling the absorber dynamically and to understand the dynamic behaviour of the absorber during part load operation and with disturbances from the stripper. A powerful modelling and simulation tool gPROMS was chosen to implement the proposed work. The study indicates that the rate-based model gives a better prediction of the chemical absorption process than the equilibrium-based model. The dynamic simulation of the absorber indicates normal absorber column operation could be maintained during part load operation by maintaining the ratio of the flow rates of the lean solvent and flue gas to the absorber. Disturbances in the CO₂ loading of the lean solvent to the absorber significantly affect absorber performance. Further work will extend the dynamic modelling to the stripper for whole plant analysis.     

Dynamic modelling and analysis of post-combustion CO2 chemical absorption process for coal-fired power plants

Post-combustion capture by chemical absorption using MEA solvent remains the only commercial technology for large scale CO₂ capture for coal-fired power plants. This paper presents a study of the dynamic responses of a post-combustion CO₂ capture plant by modelling and simulation. Such a plant consists mainly of the absorber (where CO₂ is chemically absorbed) and the regenerator (where the chemical solvent is regenerated). Model development and validation are described followed by dynamic analysis of the absorber and regenerator columns linked together with recycle. The gPROMS (Process Systems Enterprise Ltd.) advanced process modelling environment has been used to implement the proposed work. The study gives insights into the operation of the absorber-regenerator combination with possible disturbances arising from integrated operation with a power generation plant. It is shown that the performance of the absorber is more sensitive to the molar L/G ratio than the actual flow rates of the liquid solvent and flue gas. In addition, the importance of appropriate water balance in the absorber column is shown. A step change of the reboiler duty indicates a slow response. A case involving the combination of two fundamental CO₂ capture technologies (the partial oxyfuel mode in the furnace and the post-combustion solvent scrubbing) is studied. The flue gas composition was altered to mimic that observed with the combination. There was an initial sharp decrease in CO₂ absorption level which may not be observed in steady-state simulations.     

Dynamic modeling and simulation of absorption of carbon dioxide into seawater

In order to elucidate the dynamic performance of the CO₂ ocean disposal process, effects of operating parameters, such as gas flow rate, salinity and temperature, on the absorption of CO₂ into seawater were examined. The rate-based model consisting of the rates of chemical reaction and gas-liquid mass transfer was developed for simulating dynamic process of CO₂ ocean disposal. In modeling, non-ideal mixing characteristics in the gas and liquid phases are described using a tanks-in-series model with backflow. Experiments were performed to verify dynamic CO₂ absorption prediction capability of the proposed model in a cylindrical bubble column. The operation was batch and continuous with respect to liquid phase and gas phase, respectively. Experimental results indicate that the CO₂ gas injection rate increased the absorption rate but the increase in salinity concentration caused inhibition of the absorption of CO₂. The proposed model could describe the present experimental results for the dynamic changes and the steady-state values of dissolved CO₂ concentration and hydrogen ion concentration. The proposed model might effectively handle the prediction of the absorption of CO₂ into seawater in the CO₂ ocean disposal.     

Results from trialling aqueous NH3 based post-combustion capture in a pilot plant at Munmorah power station: Absorption

Australia's Commonwealth Scientific and Industrial Research Organization (CSIRO) and Delta Electricity have developed, commissioned and operated an A$7 million aqueous NH₃ based post-combustion capture (PCC) pilot plant at the Munmorah black coal fired power station in Australia. The results from the pilot plant trials will be used to address the gap in know-how on application of aqueous NH₃ for post-combustion capture of CO₂ and other pollutants in the flue gas and explore the potential of the NH₃ process for application in the Australia power sector. This paper is one of a series of publications to report and discuss the experimental results obtained from the pilot plant trials and primarily focuses on the absorption section.The pilot plant trials have confirmed the technical feasibility of the NH₃ based capture process. CO₂ removal efficiency of more than 85% can be achieved even with low NH₃ content of up to 6 wt%. The NH₃ process is effective for SO₂ but not for NO in the flue gas. More than 95% of SO₂ in the flue gas is removed in the pre-treatment column using NH₃. The mass transfer coefficients for CO₂ in the absorber as functions of CO₂ loading and NH₃ concentration have been obtained based on pilot plant data.     

Dynamic analysis of the absorption/desorption loop of a carbon capture plant using an object-oriented approach

Post-combustion capture of CO₂ is regarded as a possible technology in order to reduce CO₂ emission to the atmosphere. This paper provides a dynamic analysis of the absorption/desorption loop of a carbon capture plant with the help of a simulation model, built using the object-oriented Modelica Library Thermal Separation. The solvent used is an amino-acid salt.The dynamic behaviour is investigated for a reduction in regeneration heat flow rate but constant flue gas flow rate. Hereby four different control strategies are compared, one keeping the lean solvent loading constant, one keeping the solvent flow rate constant, one where flue gas bypasses the capture plant and a last one where an additional solvent tank is introduced. The simulation shows i.e. that for a constant lean solvent loading the response of the absorbed CO₂ flow rate is much faster than for a constant solvent flow rate.Also the effect on the dynamic behaviour is investigated, comparing the whole cycle model to a stand-alone desorber model and to a stand-alone absorber model respectively. It was found that the dynamic responses on a short time scale are very similiar, but different on a long time scale.     

Numerical Study of the CO2 Absorber Performance Subjected to the Varying Amine Solvent and Flue Gas Loads

The paper is devoted to the amine-based post-combustion carbon dioxide capture technology. The aim of the paper was to analyze the effect of varying flow conditions on the CO₂ capture efficiency of the absorber column. As a research tool, a numerical model of the chemical absorption with aqueous monoethanolamine solution in a packed bed was employed. A complex physio-chemical process including two-phase flow hydrodynamics, heat transfer, and absorption chemistry was simulated by Ansys Fluent commercial software. The parametric study was focused on CO₂ capture efficiency in terms of varying loads of amine solvent (liquid) and flue gas. The corresponding changes of liquid holdup, species concentration, temperature and reaction rate distributions are discussed in detail allowing to better understand the absorption column operation. The simulation results have shown clearly the mutual interactions of partial processes and the sensitivity of the system to varying column loads. They have been found to be useful in defining the optimal ranges of operational parameters.     

Techno-economic modelling and cost functions of CO2 capture processes

The paper presents the techno-economic modelling of CO₂ capture process in coal-fired power plants. An overall model is being developed to compare carbon capture and sequestration options at locations within the UK, and for studies of the sensitivity of the cost of disposal to changes in the major parameters of the most promising solutions identified. Technological options of CO₂ capture have been studied and cost estimation relationships (CERs) for the chosen options calculated. Created models are related to the capital, operation and maintenance cost. A total annualised cost of plant electricity output and amount of CO₂ avoided have been developed. The influence of interest rates and plant life has been analysed as well. The CERs are included as an integral part of the overall model.     

Multi-field synergy study of CO2 capture process by chemical absorption

Carbon dioxide capturing from the flue gas of power stations is an effective way to mitigate the global warming. In order to predict the performance from startup to stable operation in CO₂ absorption process, a multi-field synergy model was developed based on CO₂ capture process in a packed column by means of monoethanolamine (MEA). The model suggests that the integral diffusion–reaction coefficient plays an important role in the diffusion, fluid flow, heat transfer and chemical reaction processes. The influences of the fluid flow, heat transfer and chemical reaction can be justified using corresponding synergy numbers, quantifying multi-field interactive dynamic characteristics of the CO₂ capture process. The simulation shows a good agreement compared with data in the literature. The results show that the packing Reynolds number can be used as a criterion to choose the proper packing. The less the Reynolds number is, the more efficient the reaction absorption is. The average synergy number F_dc would be decreased by 20% with 6 K temperature drop and be descended by 7% with the 2.5% solvent weight percentage increment, which improved the efficiency of CO₂ capture by about 5% and 14%, and lowered the energy consumption by about 5%. The average synergy number F_dh would be decreased by about 8% with the 0.062 mol/molMEA lean solvent loading increment, which improved the efficiency by about 15% and lowered the energy consumption by 5%. After comparing with CMR-2, Raschig rings, Berl saddles and Pall rings, the 33% less average synergy number F_df of the CMR-2 packing with about 5% drop in energy consumption yields the highest efficiency of 71%, which is 10% higher than that of the Berl saddle packing. The results indicate that the proposed multi-field synergy model is an effective way to intensify the capture process as a guideline with the priority of precision and simplicity.     

CO2 Capture Using Monoethanolamine in a Bubble‐Column Scrubber

A continuous bubble‐column scrubber, capturing CO₂ gas by monoethanolamine (MEA) solution in a pH‐stat operation, is used to search for optimum process parameters by means of the Taguchi method. The process variables are the pH of the solution, gas flow rate, concentration of CO₂ gas, and temperature. From the measured outlet CO₂ gas concentrations, the absorption rate and overall mass transfer coefficient can be determined with the support of a steady‐state material balance equation as well as a two‐film model. According to the signal‐to‐noise ratio, the significance sequence influencing the parameters and optimum conditions can be determined. CO₂ concentration and pH value proved to be decisive parameters, while temperature and gas flow rate were minor. Five sets of optimum conditions were obtained and could be further verified by empirical equations.     

Behaviour of absorption/stripping columns for the CO2-MEA system; Modelling and experiments

A model is presented for the steady-state simulation of a CO₂ recovery pilot plant with aqueous monoethanolamine (MEA) solutions. CO₂ absorption is performed in a column packed with 2.54 cm ceramic Pall rings. CO₂ recovery is achieved in a 20 sieve tray steam stripping column. The packed column absorption model was fitted to the experimental data using the specific interfacial area of the irrigated packing as an adjustable parameter. The equivalent average bubble diameter was used as the adjusting parameter in the sieve tray stripping column. Modelling of both towers reproduces within 3% average error concentrations measured in a pilot plant. Measured temperatures were also well correlated.     

Mass transfer investigation and operational sensitivity analysis of amine-based industrial CO2 capture plant

In this article, the industrial process of CO₂ capture using monoethanolamine as an aqueous solvent was probed carefully from the mass transfer viewpoint. The simulation of this process was done using Rate-Base model, based on two-film theory. The results were validated against real plant data. Compared to the operational unit, the error of calculating absorption percentage and CO₂ loading was estimated around 2%. The liquid temperature profiles calculated by the model agree well with the real temperature along the absorption tower, emphasizing the accuracy of this model. Operational sensitivity analysis of absorption tower was also done with the aim of determining sensitive parameters for the optimized design of absorption tower and optimized operational conditions. Hence, the sensitivity analysis was done for the flow rate of gas, the flow rate of solvent, flue gas temperature, inlet solvent temperature, CO₂ concentration in the flue gas, loading of inlet solvent, and MEA concentration in the solvent. CO₂ absorption percentage, the profile of loading, liquid temperature profile and finally profile of CO₂ mole fraction in gas phase along the absorption tower were studied. To elaborate mass transfer phenomena, enhancement factor, interfacial area, molar flux and liquid hold up were probed. The results show that regarding the CO₂ absorption, the most important parameter was the gas flow rate. Comparing liquid temperature profiles showed that the most important parameter affecting the temperature of the rich solvent was MEA concentration.     

Modelling reactive absorption of CO2 in packed columns for post-combustion carbon capture applications

A rate-based process model for the reactive absorption of carbon dioxide (CO₂) from a gas mixture into an aqueous monoethanolamine (MEA) solution in a packed column is developed. The model is based on the fast second-order kinetics for the CO₂-MEA reactions and takes into account the mass transfer resistances. The heat effects associated with the absorption and chemical reaction are included through energy balances in the gas and liquid phases. Appropriate correlations for the key thermodynamic and transport properties and for the gas-liquid mass transfer are incorporated into the model to ensure reliable predictions. The model predictions are validated by simulating a series of experiments conducted in pilot and industrial scale absorption columns with random and structured packings reported in the literature. Comparisons between the simulation results and the experimental data reveal good quality predictions of the gas phase CO₂ and MEA concentrations and the liquid temperature along the column height. The sensitivity studies reveal that the correlations for the gas- and liquid-film mass transfer coefficients given by Onda et al. (1968) provide better predictions than the penetration theory of Higbie (1935) and the correlation of Bravo et al. (1985).     

Numerical Simulation of Absorbing CO2 with Ionic Liquids

Although separating CO₂ from flue gas with ionic liquids has been regarded as a new and effective method, the mass transfer properties of CO₂ absorption in these solvents have not been researched. In this paper, a coupled computational fluid dynamic (CFD) model and population balance model (PBM) was applied to study the mass transfer properties for capturing CO₂ with ionic liquids solvents. The numerical simulation was performed using the Fluent code. Considering the unique properties of ionic liquids, the Eulerian‐Eulerian two‐flow model with a new drag coefficient correlation was employed for the gas‐liquid fluid dynamic simulation. The gas holdup, interfacial area, and bubble size distribution in the bubble column reactor were predicted. The mass transfer coefficients were estimated with Higbie's penetration model. Furthermore, the velocity field and pressure field in the reactor were also predicted in this paper.     

Removal of carbon dioxide from flue gases in packed column using ionic liquids

The study of CO₂ absorption in ionic liquids (ILs): [Emim] [Ac], [Bmim] [Ac] in a packed column is presented. The influence of mass transfer resistances, initial CO₂ concentration, absorption temperature and 2, 5, 10% wt. water addition on CO₂ removal efficiency was investigated. The resistance in series model and estimated values of enhancement factor were used to predict with good accuracy mass fluxes of absorbed carbon dioxide for both ILs. The CO₂ absorption efficiency in packed column depends on temperature and initial CO₂ concentration. The addition of small amounts of water to [Emim][Ac] is of minor effect on CO₂ absorption.     

Efficient capture of carbon dioxide with novel mass‐transfer intensification device using ionic liquids

A novel mass‐transfer intensified approach for CO₂ capture with ionic liquids (ILs) using rotating packed bed (RPB) reactor was presented. This new approach combined the advantages of RPB as a high mass‐transfer intensification device for viscous system and IL as a novel, environmentally benign CO₂ capture media with high thermal stability and extremely low volatility. Amino‐functionalized IL (2‐hydroxyethyl)‐trimethyl‐ammonium (S)?2‐pyrrolidinecarboxylic acid salt ([Choline][Pro]) was synthesized to perform experimental examination of CO₂ capture by chemical absorption. In RPB, it took only 0.2 s to reach 0.2 mol CO₂/mol IL at 293 K, indicating that RPB was kinetically favorable to absorption of CO₂ in IL because of its efficient mass‐transfer intensification. The effects of operation parameters on CO₂ removal efficiency and IL absorbent capacity were studied. In addition, a model based on penetration theory was proposed to explore the mechanism of gas–liquid mass transfer of ILs system in RPB. © 2013 American Institute of Chemical Engineers AIChE J, 59: 2957–2965, 2013     

Absorption of carbon dioxide into aqueous blends of 2-amino-2-methyl-1-propanol and monoethanolamine

This work presents an investigation of CO₂ absorption into aqueous blends of 2-amino-2-methyl-1-propanol (AMP) and monoethanolamine (MEA). The acid gas mass transfer has been modeled using equilibrium-mass transfer-kinetics-based combined model to describe CO₂ absorption into the amine blends according to Higbie's penetration theory. The effect of contact time and relative amine concentration on the rate of absorption and enhancement factor were studied by absorption experiment in a wetted wall column at atmospheric pressure. The model was used to estimate the rate coefficient of the reaction between CO₂ and monoethanolamine at 313 K from experimentally measured absorption rates. A rigorous parametric sensitivity test has been done to identify the key systems’ parameters and quantify their effects on the mass transfer using the mathematical model developed in this work. The model predictions have been found to be in good agreement with the experimental rates of absorption of CO₂ into (AMP+MEA+H₂O).     

Rheological,Thermodynamic, and Gas Solubility Properties of Phenylacetic Acid‐Based Deep Eutectic Solvents

Choline chloride + phenylacetic acid‐based deep eutectic solvents are studied. Their most relevant experimental physicochemical properties at different mixing ratios together with the CO₂ solubility data obtained in wide pressure and temperature ranges are reported. The presented materials exhibit a significant CO₂ capture performance with low corrosion effect when compared with the most common amine‐based CO₂ capture agents. Detailed rheological measurements are carried out and various models are applied to describe the dynamic flow behavior of the solvents. The CO₂ absorption mechanism is evaluated by studying the behavior of the liquid gas and interface. Due to the advantages of low cost, nontoxicity, and favorable physical properties, these solvents are an environmentally promising alternative for effective CO₂ capture technological applications.