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See detailInfluence of process operating conditions on solvent thermal and oxidative degradation in post-combustion CO2 capture
Léonard, Grégoire ULg; Crosset, Cyril; Toye, Dominique ULg et al

in Computers & Chemical Engineering (in press)

///Document soumis, la révision doit encore être faite./// The CO2 post-combustion capture with amine solvents is modeled as a complex system interconnecting process energy consumption and solvent ... [more ▼]

///Document soumis, la révision doit encore être faite./// The CO2 post-combustion capture with amine solvents is modeled as a complex system interconnecting process energy consumption and solvent degradation and emission. Based on own experimental data, the kinetics of monoethanolamine degradation is included into a model of the CO2 capture process. The influences of operating conditions and flowsheet improvements on solvent loss and process energy requirement are quantified and validated with pilot plant data. Oxidative degradation in the absorber is identified as the major cause of solvent loss. On the contrary, thermal degradation does not appear as a major concern. Finally, this study leads to a decrease by 10% of the process exergy requirement along with a reduction by 11% of the solvent loss, all that by using a single model. Thus, this model provides a practical tool to minimize both the energy requirement and the solvent degradation by the design of large-scale CO2 capture units. [less ▲]

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See detailCarbon capture and storage at the University of Liège
Léonard, Grégoire ULg

Scientific conference (2014, November 05)

The objective of this presentation was to discuss the main technologies of CO2 capture, re-use and storage, with their respective characteristics (costs, challenges...), advantages and drawbacks. Then ... [more ▼]

The objective of this presentation was to discuss the main technologies of CO2 capture, re-use and storage, with their respective characteristics (costs, challenges...), advantages and drawbacks. Then, the second part of the presnetation highlights the main research results that have been achieved at the University of Liège in this field. [less ▲]

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See detailDesigning large-scale CO2 capture units with assessment of solvent degradation
Léonard, Grégoire ULg; Crosset, Cyril; Dumont, Marie-Noëlle ULg et al

Poster (2014, October)

Solvent degradation is a major drawback for the large-scale implementation of post-combustion CO2 capture due to amine consumption and emission of degradation products. In the present work, we refine a ... [more ▼]

Solvent degradation is a major drawback for the large-scale implementation of post-combustion CO2 capture due to amine consumption and emission of degradation products. In the present work, we refine a previous kinetic model for describing solvent oxidative and thermal degradation based on experimental results. The CO2 capture process is then modeled in Aspen Plus with assessment of solvent degradation. As a result, this work provides a useful tool for the identification of optimal operating conditions that minimize both the energy and environmental impacts of the process. [less ▲]

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See detailAssessment of Solvent Degradation within a Global Process Model of Post-Combustion CO2 Capture
Léonard, Grégoire ULg; Heyen, Georges ULg; Toye, Dominique ULg

Conference (2014, June 17)

Solvent degradation may be a major drawback for the large-scale implementation of post-combustion CO2 capture due to amine consumption and emission of degradation products. However, its influence on the ... [more ▼]

Solvent degradation may be a major drawback for the large-scale implementation of post-combustion CO2 capture due to amine consumption and emission of degradation products. However, its influence on the process operations has rarely been studied. In the present work, a kinetics model describing solvent oxidative and thermal degradation has been developed based on own experimental results for the benchmark solvent, i.e. 30 wt% monoethanolamine (MEA) in water. This model has been included into a global Aspen Plus model of the CO2 capture process. The selected process modelling approaches are described in the present work. Using the resulting simulation model, optimal operating conditions can be identified to minimize both the energy requirement and the solvent degradation in the process. This kind of process model assessing solvent degradation may contribute to the design of large-scale CO2 capture plants to consider not only the process energy penalty, but also its environmental penalty. Indeed, both aspects are relevant for the large-scale deployment of the CO2 capture technology. [less ▲]

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See detailCapture, utilisation et stockage du CO2
Léonard, Grégoire ULg

Scientific conference (2014, February)

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See detailDesigning large-scale CO2 capture units with assessment of solvent degradation
Léonard, Grégoire ULg; Crosset, Cyril; Dumont, Marie-Noëlle ULg et al

in Energy Procedia (2014), 63

Solvent degradation is one of the main operational drawbacks of post-combustion CO2 capture with amine solvents. Although the different degradation mechanisms have been largely studied in recent years, it ... [more ▼]

Solvent degradation is one of the main operational drawbacks of post-combustion CO2 capture with amine solvents. Although the different degradation mechanisms have been largely studied in recent years, it is still impossible to predict the solvent losses and the emissions of degradation products that may occur in a CO2 capture plant depending on its size and on its operating conditions. In the present work, we experimentally study the degradation of MEA monoethanolamine) under accelerated conditions implying high temperature, continuous gas feed and vigorous agitation. A special focus is set on the oxidative degradation of MEA, which is studied in the absence of CO2. Based on the experimental results, we propose a kinetic model to describe both MEA oxidative and thermal degradation pathways. The degradation kinetics is then included into a global model of the CO2 capture process, enabling solvent losses and emissions of degradation products to be predicted as a function of the process operating conditions. The predicted MEA loss is in the same order of magnitude as reported in degradation measurements from pilot plants, although lower by a factor 3. This kind of model assessing solvent degradation could and should be used for the design of large-scale CO2 capture plants in order to simultaneously consider the energy consumption of the process and its environmental impact related to the emissions of degradation products and amine solvent. Further developments shall consider the effect of SOx, NOx and dissolved metals on MEA degradation. [less ▲]

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See detailInfluence of dissolved metals and oxidative degradation inhibitors on the oxidative and thermal degradation of monoethanolamine in post-combustion CO2 capture
Léonard, Grégoire ULg; Voice, Alexander; Toye, Dominique ULg et al

in Industrial and Engineering Chemistry Reseach (2014), 53(47), 18121

In the present work, the influence of metal ions and oxidative degradation inhibitors on the stability of monoethanolamine solvents (MEA) is studied. Solvent degradation induces additional costs and ... [more ▼]

In the present work, the influence of metal ions and oxidative degradation inhibitors on the stability of monoethanolamine solvents (MEA) is studied. Solvent degradation induces additional costs and impacts the environmental balance of the CO2 capture process as well as its efficiency. The two main degradation pathways of MEA are studied under accelerated conditions: oxidative degradation with continuous gas feed and thermal degradation in batch reactors. It is confirmed that metal ions (resulting from solvent impurities and wall leaching) enhance the oxidative degradation of MEA, while they do not impact its thermal degradation. Moreover, different oxidative degradation inhibitors are tested with varying results according to the inhibitor. It appears that at the selected concentration, radical scavengers like Inhibitor A and DMTD (2,5-dimercapto-1,3,4-thiadiazole) are more efficient than chelating agents like HEDP (1-hydroxyethylidene diphosphonic acid) at inhibiting oxidative degradation. Furthermore, attention must be paid to the influence of oxidative degradation inhibitors on the thermal degradation of MEA. Indeed, some inhibitors like DMTD, DTPA (diethylenetriaminepentaacetic acid), and DTDP (3,3′-dithiodipropionic acid) appeared to decrease the MEA thermal stability, which cannot be accepted in industrial applications. Finally, a further drawback of DTPA is its high affinity for metal ions, leading to a more corrosive solution, so its use is not recommended for CO2 capture applications. [less ▲]

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See detailExperimental study and kinetic model of monoethanolamineoxidative and thermal degradation for post-combustion CO2 capture
Léonard, Grégoire ULg; Toye, Dominique ULg; Heyen, Georges ULg

in International Journal of Greenhouse Gas Control (2014), 30

In the present work, a kinetic model is proposed for the prediction of amine solvent degradation in the post-combustion CO2 capture process. Solvent degradation combined to the emission of degradation ... [more ▼]

In the present work, a kinetic model is proposed for the prediction of amine solvent degradation in the post-combustion CO2 capture process. Solvent degradation combined to the emission of degradation products represents one of the main operational drawbacks of this process. It induces additional costsand it impacts the process efficiency and its environmental balance. In the present work, degradation isstudied under accelerated conditions for the case of monoethanolamine solvent (MEA). The influence of the temperature and of the O2 and CO2 concentrations in the gas feed are studied, and their effect on theMEA loss and the emission of degradation products is quantified. Based on the experimental results, a kinetic model for both oxidative and thermal degradation of MEA is proposed and compared to previous attempts to model MEA degradation. The present kinetic model may be further used to develop a practical tool assessing solvent degradation in large-scale capture plants. [less ▲]

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See detailRelevance of accelerated conditions for the study of monoethanolamine degradation in post-combustion CO2 capture.
Léonard, Grégoire ULg; Toye, Dominique ULg; Heyen, Georges ULg

in Canadian Journal of Chemical Engineering (2014), 93(2), 348

Solvent degradation represents one of the main operational drawbacks of the post-combustion CO2 capture process. Degradation not only induces additional costs for solvent make-up, it also impacts the ... [more ▼]

Solvent degradation represents one of the main operational drawbacks of the post-combustion CO2 capture process. Degradation not only induces additional costs for solvent make-up, it also impacts the process efficiency and its environmental penalty due to the emission of various degradation products. There is still a gap of knowledge about the influence of process operating conditions on degradation, making it currently impossible to predict the solvent degradation rate in CO2 capture plants. Morever, the reaction mechanisms corresponding to solvent degradation are very slow, significantly complicating its study in industrial units. In the present work, appropriate experimental equipment and analytical methods are developed for accelerating the degradation of monoethanolamine solvents (MEA). The relevance of accelerated conditions is established by comparing artificially degraded solvent samples with degraded solvent samples from industrial CO2 capture pilot plants. Two approaches are evaluated implying either discontinuous or continuous gas feed, this latest being the most representative of industrial degradation. The respective influences of the gas feed composition and the gas-liquid transfer are evidenced and quantified. Finally, the present study leads to a better understanding of solvent degradation in the CO2 capture process with MEA. More generally, it also evidences that accelerated conditions at laboratory-scale may provide relevant information for the study of slow phenomena taking place in large-scale industrial processes. Further works include the development of a kinetic model for MEA solvent degradation and the extension of this methodology to other promising solvents in order to facilitate the operation and large-scale deployment of CO2 capture. [less ▲]

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See detailAssessment of Solvent Degradation within a Global Process Model of Post-Combustion CO2 Capture
Léonard, Grégoire ULg; Toye, Dominique ULg; Heyen, Georges ULg

in Computer Aided Chemical Engineering (2014), 33

Solvent degradation may be a major drawback for the large-scale implementation of post-combustion CO2 capture due to amine consumption and emission of degradation products. However, its influence on the ... [more ▼]

Solvent degradation may be a major drawback for the large-scale implementation of post-combustion CO2 capture due to amine consumption and emission of degradation products. However, its influence on the process operations has rarely been studied. In the present work, a kinetics model describing solvent oxidative and thermal degradation has been developed based on own experimental results for the benchmark solvent, i.e. 30 wt% monoethanolamine (MEA) in water. This model has been included into a global Aspen Plus model of the CO2 capture process. The selected process modelling approaches are described in the present work. Using the resulting simulation model, optimal operating conditions can be identified to minimize both the energy requirement and the solvent degradation in the process. This kind of process model assessing solvent degradation may contribute to the design of large-scale CO2 capture plants to consider not only the process energy penalty, but also its environmental penalty. Indeed, both aspects are relevant for the large-scale deployment of the CO2 capture technology. [less ▲]

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See detailModeling post-combustion CO2 capture with assessment of solvent degradation
Léonard, Grégoire ULg; Belletante, Ségolène; Cabeza Mogador, Bruno et al

Conference (2013, October)

Post-combustion CO2 capture in power plants is one of the most mature technologies for a short-term and large-scale decrease of CO2 emissions while simultaneously addressing the growing global energy ... [more ▼]

Post-combustion CO2 capture in power plants is one of the most mature technologies for a short-term and large-scale decrease of CO2 emissions while simultaneously addressing the growing global energy demand. CO2 is chemically absorbed in an amine solvent that can be regenerated at higher temperature, producing a pure CO2 stream. However, the large impact of this technology on the power plant efficiency and the environmental penalty are the main drawbacks for large-scale implementation. In this work, an innovative approach combining process modeling and evaluation of the environmental penalty due to amine degradation is presented. Based on experimental results, the kinetics of solvent oxidative and thermal degradation is estimated and included in the process model developed in Aspen Plus. Using this model, the influence of operating parameters like the oxygen concentration in the flue gas or the solvent regeneration pressure is studied. This model is a first step for a multi-objective optimization of the CO2 capture process, assessing both energy and environmental penalties of this technology. [less ▲]

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See detailOptimal conception of a post-combustion CO2 capture unit with assessment of solvent degradation
Léonard, Grégoire ULg; Toye, Dominique ULg; Heyen, Georges ULg

Poster (2013, September)

Solvent degradation may be a major drawback for the large-scale implementation of post-combustion CO2 capture due to amine consumption and emission of degradation products. A kinetics model describing ... [more ▼]

Solvent degradation may be a major drawback for the large-scale implementation of post-combustion CO2 capture due to amine consumption and emission of degradation products. A kinetics model describing solvent oxidative and thermal degradation has been developed based on experimental results. This model has been included into a global Aspen Plus model of the CO2 capture process, so that optimal operating conditions can be identified to minimize both energy and environmental impacts of the process. [less ▲]

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See detailOptimal design of a CO2 capture unit with assessment of solvent degradation
Léonard, Grégoire ULg

Doctoral thesis (2013)

CO2 capture in power plants by absorption in amine solvents is a technology aiming at the reduction of CO2 emissions while simultaneously addressing the growth of the global energy demand. However, the ... [more ▼]

CO2 capture in power plants by absorption in amine solvents is a technology aiming at the reduction of CO2 emissions while simultaneously addressing the growth of the global energy demand. However, the energy impact of this technology on the power plant efficiency is high and amine solvent degradation induces a non-negligible environmental impact. The main innovation of this thesis is to combine both aspects within a process model based on experimental data of solvent degradation. This model leads to the identification of optimal operating conditions for the CO2 capture process, from an energetic as well as environmental point of view. [less ▲]

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See detailDynamic Modeling and control of a pilot CO2 postcombustion capture plant
Léonard, Grégoire ULg; Cabeza Mogador, Bruno; Belletante, Ségolène et al

Poster (2013, June)

A dynamic model of a post-combustion capture pilot plant is developed using Aspen Plus Dynamics. An innovative process control strategy is studied for regulating the water balance of the process. A ... [more ▼]

A dynamic model of a post-combustion capture pilot plant is developed using Aspen Plus Dynamics. An innovative process control strategy is studied for regulating the water balance of the process. A washing section where the flue gas from the absorber is washed with cold water is included to the process in order to reduce the emissions of amine to the air. Control of the water balance in the solvent loop is successfully achieved by changing the washing water temperature. In previous publications regarding CO2 capture pilot plants, the regulation of the water balance always required a water make-up flow which appears here as unnecessary. Rejection of disturbances and different load reduction scenarios are tested to confirm the efficiency of this strategy. Potential operational problems of this control strategy are identified and solved. [less ▲]

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See detailProgress Report February 2013
Léonard, Grégoire ULg

E-print/Working paper (2013)

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See detailCapture, Utilisation et Stockage du CO2
Léonard, Grégoire ULg

Scientific conference (2013, February)

Présentation des différentes techniques de capture du CO2, des principales voies de valorisation et de la technologie de stockage sous-terrain du CO2.

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See detailDynamic modelling and control of a pilot plant for post-combustion CO2 capture
Léonard, Grégoire ULg; Cabeza Mogador, Bruno; Belletante, Ségolène et al

in Computer Aided Chemical Engineering (2013), 31

A dynamic model of a post-combustion pilot capture plant is developed using Aspen Plus Dynamics. An innovative process control strategy is studied for regulating the water balance of the process. A ... [more ▼]

A dynamic model of a post-combustion pilot capture plant is developed using Aspen Plus Dynamics. An innovative process control strategy is studied for regulating the water balance of the process. A washing section where the flue gas from the absorber is washed with cold water is included to the process in order to reduce the emissions of amine to the air. Control of the water balance in the solvent loop is successfully achieved by changing the washing water temperature. In previous publications regarding CO2 capture pilot plants, the regulation of the water balance always required a water make-up flow which appears here as unnecessary. Rejection of disturbances and different load reduction scenarios are tested to confirm the efficiency of this strategy. Potential operational problems of this control strategy are identified and solved. [less ▲]

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See detailModélisation du captage post-combustion du CO2 avec évaluation de la dégradation des solvants
Léonard, Grégoire ULg; BELLETANTE, Ségolène; Cabeza Mogador, Bruno et al

in Récents Progrès en Génie des Procédés (2013), 104

Post-combustion CO2 capture in power plants is one of the most mature technologies for a short-term and large-scale decrease of CO2 emissions while simultaneously addressing the growing global energy ... [more ▼]

Post-combustion CO2 capture in power plants is one of the most mature technologies for a short-term and large-scale decrease of CO2 emissions while simultaneously addressing the growing global energy demand. CO2 is chemically absorbed in an amine solvent that can be regenerated at higher temperature, producing a pure CO2 stream. However, the large impact of this technology on the power plant efficiency and the environmental penalty are the main drawbacks for large-scale implementation. In this work, an innovative approach combining process modeling and evaluation of the environmental penalty due to amine degradation is presented. Based on experimental results, the kinetics of solvent oxidative and thermal degradation is estimated and included in the process model developed in Aspen Plus. Using this model, the influence of operating parameters like the oxygen concentration in the flue gas or the solvent regeneration pressure is studied. This model is a first step for a multi-objective optimization of the CO2 capture process, assessing both energy and environmental penalties of this technology. [less ▲]

Detailed reference viewed: 70 (11 ULg)
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See detailProgress Report December 2012
Léonard, Grégoire ULg

E-print/Working paper (2012)

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See detailCO2 CAPTURE in POWER PLANTS: Process Simulation and Solvent Degradation
Léonard, Grégoire ULg; Lepaumier, Hélène; Thielens, Marie-Laure et al

Poster (2012, November)

Presentation of the research themes studied at the University of Liège in the field of CO2 capture

Detailed reference viewed: 27 (1 ULg)