Fundamental studies of carbon dioxide capture and conversion – computational insights into CO2 binding and catalysis

Abstract

The continuous rise in atmospheric CO2 concentrations poses a severe environmental challenge, necessitating the development of efficient CO2 capture technologies. Although amine-based solvents remain the dominant method in industrial applications, their high energy consumption and corrosive nature limit their widespread adoption. Consequently, ionic liquids (ILs) and deep eutectic solvents (DESs) have attracted significant attention as alternative solvents due to their tunable properties, low volatility, and excellent CO2 absorption capacity. ILs have demonstrated outstanding performance in CO2 capture, particularly when functionalized to enhance their chemical interactions with CO2. However, their high viscosity, toxicity, and cost remain significant challenges for industrial applications. In contrast, DESs, especially functionalized and natural DESs, are considered more sustainable alternatives due to their low toxicity, biodegradability, and cost-effectiveness. Moreover, compared to CO2 capture, CO2 conversion presents a more promising approach. Converting CO2 into value-added chemicals not only mitigates the environmental impact of CO2 emissions but also reduces dependence on fossil resources. Computational studies, including density functional theory (DFT) and molecular dynamics (MD) simulations, play a crucial role in elucidating the fundamental interactions between CO2 and both solvents and catalysts, providing essential guidance for the rational design of new materials. In this study, MD and DFT methodologies were employed to investigate CO2 adsorption behavior in natural DESs and to explore the CO2 reduction mechanisms of three molecular catalysts based on inexpensive iron metals : an Iron(II)-scorpionate catalyst and two iron porphyrin catalysts. By offering in-depth insights into CO2 adsorption and catalytic properties, this research provides a theoretical foundation for the design of highly efficient CO2 capture solvents and conversion catalysts.

Date of Award	24 Jun 2025
Original language	English
Awarding Institution	The University of Manchester
Supervisor	Carmine D'Agostino (Supervisor), Samuel De Visser (Supervisor), Paola Carbone (Supervisor) & Chris Hardacre (Supervisor)