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Mechanisms of CO2 Absorption in Amino Acid-Based Deep Eutectic Solvents: Insights from Molecular Dynamics and DFT Calculations.

Created on 29 May 2025

Authors

Hung-Yi Chi, Heng-Kwong Tsao, Yu-Jane Sheng

Published in

The journal of physical chemistry. B. May 28, 2025. Epub May 28, 2025.

Abstract

This study explores the mechanisms of CO2 absorption in two amino acid-containing deep eutectic solvents (DESs) through molecular dynamics (MD) simulations and density functional theory (DFT) calculations. The MD simulations, which focus mainly on physical absorption, reveal that alanine-based DES (Ala DES) exhibits higher CO2 solubility than l-arginine-based DES (l-arg DES), attributed to stronger physical absorption. Furthermore, the hydrogen bond donor paired with the amino acids is identified as a critical factor for enhancing physical absorption efficiency. DFT calculations, which account for chemical absorption, investigate two reaction pathways: single-molecule reactions involving intramolecular proton transfer and two-molecule reactions involving intermolecular proton exchange. While Ala DES does not exhibit spontaneous chemical absorption, l-arg DES demonstrates such reactions, leading to the formation of carbamic acid or carbamate (ΔG < 0), indicative of CO2 capture through chemical interactions. Consequently, Ala DES primarily relies on physical absorption, whereas l-arg DES utilizes multiple reactive sites for chemical absorption. These results are consistent with experimental findings, which show that l-arg DES achieves higher CO2 solubility under atmospheric conditions. Overall, our study highlights the interplay between DES components and reactivity in enhancing CO2 capture efficiency.

PMID:
40435364
Bibliographic data and abstract were imported from PubMed on 29 May 2025.

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