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Enhanced CO2 capture performance of mesoporous silica materials with TEPA amine-based deep eutectic solvent: kinetics and mechanism

Enhanced CO2 capture performance of mesoporous silica materials with TEPA amine-based deep eutectic solvent: kinetics and mechanism
Enhanced CO2 capture performance of mesoporous silica materials with TEPA amine-based deep eutectic solvent: kinetics and mechanism
Conventional amine-based sorbents exhibit two major drawbacks: progressive structural deterioration under repetitive CO2 adsorption–desorption cycling and diminished gas capture efficiency with extended cycle iterations. To mitigate these issues, a new amine-based deep eutectic solvent (DES) containing tromethamine (TrMA) salt as a sterically hindered amine and tetraethylenepentamine (TEPA) was prepared and incorporated into several mesoporous silica materials for CO2 capture, including SBA-15, SBA-16, MCM-41, and KIT-6. In comparison to SBA-16 and MCM-41 materials, SBA-15 and KIT-6 could maintain their mesoporous structure after incorporation of 50% DES, as revealed by the N2 sorption analysis. According to the findings, (50%) TrMA-TEAP (1 : 2)/SBA-15 had a higher CO2 adsorption of 120.8 (mg g−1) than (50%) pure TEAP (1 : 2)/SBA-15 and the other hybrid amine-based DES/mesoporous silica materials at 75 °C under 15% CO2 balanced N2. Furthermore, the adsorption index values for (50%) TrMA-TEAP (1 : 2)/SBA-15 and (50%) pure TEAP (1 : 2)/SBA-15 were 94.9% and 92.5%, respectively, demonstrating that amine-based DES showed superior cycle performance, albeit (50%) TrMA-TEAP (1 : 2)/KIT-6 showed an excellent cycling performance by maintaining the original CO2 adsorption capacity of 97.3%, amongst the other sorbents. Pseudo-first order, pseudo-second order, Vermeulen, Avrami, and fractal-like exponential kinetic models were used to investigate the kinetic adsorption of hybrid sorbents, with the last kinetic model offering the best fitting. The DFT analysis demonstrated that the primary amine and hydroxyl (OH) groups site on the hydrogen bond donor/acceptor (HBA) are more active site in DES, while the hydrogen bond donor (HBD) plays a dominant role in CO2 adsorption due to possessing more amine active sites, particularly primary amine sites.
2050-7488
23655-23670
Ghaedi, Hosein
aabcd409-5a73-491d-93ef-1194ea65da2d
Fu, Jiawen
62ed87b3-29a8-4076-bd44-2b937f091e8c
Kalhor, Payam
ab08ec78-2042-4beb-8dd1-5274bf91f8c7
Masoudi Soltani, Salman
c9b03403-a3a8-4f22-a87e-b55f2d492f96
Zhao, Ming
c10b3f2f-e507-410b-9e2a-1b979180d896
Ghaedi, Hosein
aabcd409-5a73-491d-93ef-1194ea65da2d
Fu, Jiawen
62ed87b3-29a8-4076-bd44-2b937f091e8c
Kalhor, Payam
ab08ec78-2042-4beb-8dd1-5274bf91f8c7
Masoudi Soltani, Salman
c9b03403-a3a8-4f22-a87e-b55f2d492f96
Zhao, Ming
c10b3f2f-e507-410b-9e2a-1b979180d896

Ghaedi, Hosein, Fu, Jiawen, Kalhor, Payam, Masoudi Soltani, Salman and Zhao, Ming (2025) Enhanced CO2 capture performance of mesoporous silica materials with TEPA amine-based deep eutectic solvent: kinetics and mechanism. Journal of Materials Chemistry A, 13 (29), 23655-23670. (doi:10.1039/D5TA02784E).

Record type: Article

Abstract

Conventional amine-based sorbents exhibit two major drawbacks: progressive structural deterioration under repetitive CO2 adsorption–desorption cycling and diminished gas capture efficiency with extended cycle iterations. To mitigate these issues, a new amine-based deep eutectic solvent (DES) containing tromethamine (TrMA) salt as a sterically hindered amine and tetraethylenepentamine (TEPA) was prepared and incorporated into several mesoporous silica materials for CO2 capture, including SBA-15, SBA-16, MCM-41, and KIT-6. In comparison to SBA-16 and MCM-41 materials, SBA-15 and KIT-6 could maintain their mesoporous structure after incorporation of 50% DES, as revealed by the N2 sorption analysis. According to the findings, (50%) TrMA-TEAP (1 : 2)/SBA-15 had a higher CO2 adsorption of 120.8 (mg g−1) than (50%) pure TEAP (1 : 2)/SBA-15 and the other hybrid amine-based DES/mesoporous silica materials at 75 °C under 15% CO2 balanced N2. Furthermore, the adsorption index values for (50%) TrMA-TEAP (1 : 2)/SBA-15 and (50%) pure TEAP (1 : 2)/SBA-15 were 94.9% and 92.5%, respectively, demonstrating that amine-based DES showed superior cycle performance, albeit (50%) TrMA-TEAP (1 : 2)/KIT-6 showed an excellent cycling performance by maintaining the original CO2 adsorption capacity of 97.3%, amongst the other sorbents. Pseudo-first order, pseudo-second order, Vermeulen, Avrami, and fractal-like exponential kinetic models were used to investigate the kinetic adsorption of hybrid sorbents, with the last kinetic model offering the best fitting. The DFT analysis demonstrated that the primary amine and hydroxyl (OH) groups site on the hydrogen bond donor/acceptor (HBA) are more active site in DES, while the hydrogen bond donor (HBD) plays a dominant role in CO2 adsorption due to possessing more amine active sites, particularly primary amine sites.

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Accepted/In Press date: 14 June 2025
e-pub ahead of print date: 16 June 2025

Identifiers

Local EPrints ID: 504152
URI: http://eprints.soton.ac.uk/id/eprint/504152
ISSN: 2050-7488
PURE UUID: c61d2893-1e74-4a10-b8bc-a00ea9b3d2a0
ORCID for Payam Kalhor: ORCID iD orcid.org/0000-0002-9140-1138

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Date deposited: 28 Aug 2025 16:30
Last modified: 29 Aug 2025 02:16

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Contributors

Author: Hosein Ghaedi
Author: Jiawen Fu
Author: Payam Kalhor ORCID iD
Author: Salman Masoudi Soltani
Author: Ming Zhao

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