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CO2 Capture Using Slurries of Immobilized Deep Eutectic Solvents: From Synthetic Gas Studies to Real Flue Gas Implementation
Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.ORCID iD: 0000-0002-8946-9491
2026 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The mitigation of anthropogenic CO2 emissions requires the development of efficient, stable, and economically viable capture technologies beyond conventional amine-based systems. Deep eutectic solvents (DESs) have emerged as promising alternatives due to their tunable properties and high CO2 affinity; however, their practical application is often limited by high viscosity and mass-transfer constraints. This study investigates the design, optimization, and validation of DES-based systems for CO2 capture, with particular emphasis on combining cosolvent addition and immobilization strategies to enhance overall performance.

In the first part, [MEACl][EDA]-based DESs with varying molar ratios were synthesized and evaluated as aqueous CO2 absorbents. An aqueous 40 wt.% [MEACl][EDA] (1:5) system was identified as optimal, exhibiting higher CO2 uptake (22.09 wt.% at 22 ºC and 1 atm), faster absorption kinetics (1.24 mol CO2/(kg sorbent·min) after 2 min at 22 ºC), and comparable viscosity (4.401 mPa·s before and 13.330 mPa·s after CO2 capture) relative to benchmark 30 wt.% aqueous monoethanolamine (MEA) (15.74 wt.% CO2 capture capacity, viscosity of 3.318 mPa·s before and 8.413 mPa·s after CO2 capture), along with good thermal stability and recyclability (~88% regeneration). To further improve performance, a novel hybrid approach was developed by immobilizing 5 wt.% DES within mesoporous silica and dispersing 3 wt.% of the composite in 40 wt.% aqueous DES to form slurries. These hybrid systems demonstrated enhanced CO2 capacity (up to 24.93 wt.% at 22 ºC and 1 atm), improved sorption rates (1.4 mol CO2/(kg sorbent·min) after 2 min at 22 ºC), and acceptable viscosity (7.32 and 21.82 mPa·s before and after CO2 capture) and cyclic stability (~91% recovery).

To study the desorption performance, the strategy was extended to non-aqueous systems by immobilizing 5 wt.% DES within mesoporous silica and dispersing 3 wt.% of the composite in 20 wt.% DES in ethylene glycol as a cosolvent, resulting in slurries with improved desorption kinetics (0.38 mol CO2/(kg sorbent·min) after 2 min at 110 ºC), superior thermal stability, minimal solvent loss, and promising regeneration performance (96.4% recovery). Finally, the practical applicability of the developed systems was validated using real biomass combustion flue gas and synthetic gas mixtures (CO2/N2 and CO2/CH4) over a wide pressure range. The aqueous DES-based systems achieved CO2 removal efficiencies >97%, whereas the non-aqueous systems reached 75-85% at 25 ºC and 1 atm for real flue gas. Pressure-dependent studies using CO2/N2 and CO2/CH4 mixtures showed enhanced CO2 uptake with increasing pressure for all systems, with aqueous slurries consistently outperforming their non-aqueous counterparts, while the latter exhibited additional CH4 uptake due to physical sorption in the ethylene glycol phase.

Place, publisher, year, edition, pages
Luleå: Luleå University of Technology, 2026.
Series
Doctoral thesis / Luleå University of Technology 1 jan 1997 → …, ISSN 1402-1544
Keywords [en]
CO2 capture, Flue gas, Deep eutectic solvent, Immobilization, Slurry
National Category
Energy Engineering
Research subject
Energy Engineering
Identifiers
URN: urn:nbn:se:ltu:diva-116522ISBN: 978-91-8048-997-3 (print)ISBN: 978-91-8048-998-0 (electronic)OAI: oai:DiVA.org:ltu-116522DiVA, id: diva2:2040720
Public defence
2026-05-11, E632, Luleå University of Technology, Luleå, 09:00 (English)
Opponent
Supervisors
Available from: 2026-02-23 Created: 2026-02-22 Last updated: 2026-02-23Bibliographically approved
List of papers
1. Reviewing and screening ionic liquids and deep eutectic solvents for effective CO2 capture
Open this publication in new window or tab >>Reviewing and screening ionic liquids and deep eutectic solvents for effective CO2 capture
2022 (English)In: Frontiers in Chemistry, E-ISSN 2296-2646, Vol. 10, article id 951951Article, review/survey (Refereed) Published
Abstract [en]

CO2 capture is essential for both mitigating CO2 emissions and purifying/conditioning gases for fuel and chemical production. To further improve the process performance with low environmental impacts, different strategies have been proposed, where developing liquid green absorbent for capturing CO2 is one of the effective options. Ionic liquids (IL)/deep eutectic solvents (DES) have recently emerged as green absorbents with unique properties, especially DESs also benefit from facile synthesis, low toxicity, and high biodegradability. To promote their development, this work summarized the recent research progress on ILs/DESs developed for CO2 capture from the aspects of those physical- and chemical-based, and COSMO-RS was combined to predict the properties that are unavailable from published articles in order to evaluate their performance based on the key properties for different IL/DES-based technologies. Finally, top 10 ILs/DESs were listed based on the corresponding criteria. The shared information will provide insight into screening and further developing IL/DES-based technologies for CO2 capture.

Place, publisher, year, edition, pages
Frontiers Media S.A., 2022
Keywords
ionic liquid, deep eutectic solvents, CO2 capture, COSMO-RS, green absorbents
National Category
Energy Engineering Other Environmental Engineering Other Chemical Engineering
Research subject
Energy Engineering
Identifiers
urn:nbn:se:ltu:diva-92835 (URN)10.3389/fchem.2022.951951 (DOI)000844308600001 ()36034653 (PubMedID)2-s2.0-85136581680 (Scopus ID)
Funder
Swedish Energy Agency
Note

Validerad;2022;Nivå 2;2022-09-07 (joosat);

Available from: 2022-09-07 Created: 2022-09-07 Last updated: 2026-02-22Bibliographically approved
2. Developing non-aqueous slurry for CO2 capture
Open this publication in new window or tab >>Developing non-aqueous slurry for CO2 capture
2025 (English)In: Carbon Capture Science and Technology, E-ISSN 2772-6568, Vol. 15, article id 100385Article in journal (Refereed) Published
Abstract [en]

The urgency of mitigating CO2 emissions has become increasingly critical due to their detrimental effects on environmental sustainability and human health. Among emerging solutions, deep eutectic solvents (DESs) have garnered attention for their high CO2 capture capacities. However, widespread application of DESs has been constrained by their inherent high viscosity and cost. To overcome these limitations, this study further explores the novel strategy, where cosolvent addition and immobilization are combined to develop a non-aqueous slurry for CO2 capture with high efficiency. Here, [MEACl][EDA] with (1:5) molar ratio is mixed with ethylene glycol (EG) to form a non-aqueous DES solution, and the DES is further immobilized into the mesoporous silica to form a composite and then mixed with the DES-EG solution to make a slurry. The CO2 capture tests demonstrated 15 wt.% capture capacity at 22 °C and 1 bar, and efficient sorption and desorption rates (0.34 and 0.38 mol CO2/(kg sorbent·min) within the initial 2 min). The slurry also exhibited promising cyclic performance with 96.4 % recovery together with minimal solvent loss of 0.97 % and almost intact structure after 120 hr of heating at 110 °C. The improved capture capacity and kinetics, especially for desorption, as well as enhanced thermal stability of the non-aqueous system highlight its potential for industrial applications.

Place, publisher, year, edition, pages
Elsevier Ltd, 2025
Keywords
Carbon capture, Deep eutectic solvent, Slurry, Immobilization, Desorption
National Category
Energy Engineering Energy Systems
Research subject
Energy Engineering
Identifiers
urn:nbn:se:ltu:diva-111667 (URN)10.1016/j.ccst.2025.100385 (DOI)001425732000001 ()2-s2.0-85217091562 (Scopus ID)
Funder
Swedish Energy Agency, 2020–90040The Swedish Foundation for International Cooperation in Research and Higher Education (STINT), CH2019–8287Swedish Research Council, 2020–03899
Note

Validerad;2025;Nivå 1;2025-03-18 (u8);

Full text license: CC BY

Available from: 2025-02-19 Created: 2025-02-19 Last updated: 2026-02-22Bibliographically approved
3. Development of Monoethanolamine Chloride-Ethylene Diamine Deep Eutectic Solvent for Ffficient Carbon Dioxide Capture
Open this publication in new window or tab >>Development of Monoethanolamine Chloride-Ethylene Diamine Deep Eutectic Solvent for Ffficient Carbon Dioxide Capture
2024 (English)In: Separation and Purification Technology, ISSN 1383-5866, E-ISSN 1873-3794, Vol. 347, article id 127593Article in journal (Refereed) Published
Abstract [en]

Deep eutectic solvents (DES) emerge as a compelling class of ionic liquids, with distinct advantages over traditional solvents, particularly in the realm of CO2 capture. In the present study, [MEACl][EDA] is synthesized across various molar ratios (1:3 to 1:10) and combined with the results of Differential Scanning Calorimetry (DSC) to identify DESs. The DESs are further characterized using Fourier Transform Infrared Spectroscopy (FTIR), and the properties and performance of the DESs with diverse water contents (30–60 wt%) are systematically studied for CO2 capture. The optimal aqueous solution is identified based on the CO2 uptake and viscosity, followed by the evaluation of the cyclic absorption experiments. Results demonstrate that 40 wt% of [MEACl][EDA] DES with (1:5) molar ratio exhibits higher CO2 uptake (22.09 wt%) and comparable viscosity (4.401 mPa·s before and 13.330 mPa·s after CO2 capture at 25 °C) compared to aqueous 40 wt% MEA (15.74 wt% CO2 capture capacity, viscosity of 3.318 mPa·s before and 8.413 mPa·s after CO2 capture), and its absorption rate is also more favorable than the aqueous MEA. Furthermore, recycling studies reveal ∼ 88 % regeneration of the aqueous DES solution at 100 °C.

Place, publisher, year, edition, pages
Elsevier, 2024
Keywords
CO2 uptake, Absorption capacity, Deep eutectic solvent, Aqueous, Regeneration
National Category
Energy Engineering
Research subject
Energy Engineering
Identifiers
urn:nbn:se:ltu:diva-105043 (URN)10.1016/j.seppur.2024.127593 (DOI)001232402700001 ()2-s2.0-85190780809 (Scopus ID)
Funder
Swedish Energy Agency, 2020-90040The Swedish Foundation for International Cooperation in Research and Higher Education (STINT), CH2019-8287Bio4EnergySwedish Research Council, 2020-03899
Note

Validerad;2024;Nivå 2;2024-05-08 (joosat);

Full text: CC BY License;

This article has previously appeared as a manuscript in a thesis.

Available from: 2024-04-09 Created: 2024-04-09 Last updated: 2026-02-22Bibliographically approved
4. Developing slurry based on immobilized and aqueous [MEACl][EDA] for CO2 capture
Open this publication in new window or tab >>Developing slurry based on immobilized and aqueous [MEACl][EDA] for CO2 capture
2024 (English)In: Chemical Engineering Journal, ISSN 1385-8947, E-ISSN 1873-3212, Vol. 499, article id 156176Article in journal (Refereed) Published
Abstract [en]

The urgent need to mitigate climate change and reduce greenhouse gas emissions has underscored the importance of developing effective CO2 capture technologies. In this study, a novel strategy was proposed and developed, where adding cosolvent and immobilizing deep eutectic solvent (DES) were combined to enhance the performance from capacity to rate. To this end, [MEACl][EDA] (1:5) was chosen as the DES, H2O was used as the cosolvent, and silica was selected as the substrate to immobilize the DES; the effects of the DES immobilization amount and the concentration of the immobilized DES particles in the aqueous system as well as temperature on the viscosity and CO2 capture performance were investigated systematically. Compared to the aqueous DES, the slurry exhibited higher CO2 uptake and improved kinetics, comparable viscosity before CO2 capture, and slightly high viscosity after CO2 capture, where the best sample (3 wt% of (5 wt% DES@silica) in 40 wt% aqueous DES) showed a capacity of 24.93 wt% at the room temperature (22 ℃) and viscosities of 7.32 and 21.82 mPa·s before and after CO2 capture. Also, the CO2 capture rate of the slurry reached 1.4 mol CO2/(kg sorbent·min) after 2 min at 22 ℃, which was higher than the aqueous DES without immobilized DES (1.24 mol CO2/(kg sorbent·min) under the same condition). The prepared slurries showed high stability (over one month) and high regeneration (∼91 % CO2 capture recovery after 5 cycles).

Place, publisher, year, edition, pages
Elsevier, 2024
Keywords
CO2 capture, Deep eutectic solvent, Slurry, Immobilization, Aqueous
National Category
Energy Engineering
Research subject
Energy Engineering
Identifiers
urn:nbn:se:ltu:diva-105044 (URN)10.1016/j.cej.2024.156176 (DOI)001328185000001 ()2-s2.0-85204968855 (Scopus ID)
Funder
Swedish Energy Agency, 2020- 90040The Swedish Foundation for International Cooperation in Research and Higher Education (STINT), CH2019-8287Bio4EnergySwedish Research Council Formas, 2020- 03899
Note

Validerad;2024;Nivå 2;2024-10-07 (sarsun);

Full text license: CC BY 4.0;

This article has previously appeared as a manuscript in a thesis;

Available from: 2024-04-09 Created: 2024-04-09 Last updated: 2026-02-22Bibliographically approved
5. Developing Slurries for Carbon Capture: From Synthetic Gas Mixtures to Real Flue Gas
Open this publication in new window or tab >>Developing Slurries for Carbon Capture: From Synthetic Gas Mixtures to Real Flue Gas
(English)Manuscript (preprint) (Other academic)
National Category
Energy Engineering
Research subject
Energy Engineering
Identifiers
urn:nbn:se:ltu:diva-116521 (URN)
Available from: 2026-02-22 Created: 2026-02-22 Last updated: 2026-03-06Bibliographically approved

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56789101110 of 11
CiteExportLink to record
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Citation style
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  • ieee
  • modern-language-association-8th-edition
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  • en-US
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