Fundamental Understanding of CO₂Capture and Regeneration in Aqueous Amines from First-Principles Studies: Recent Progress and Remaining Challenges

Abstract

Aqueous amine-based chemical scrubbing has been considered the most promising near-term solution for CO 2 capture from flue gas. However, its widespread implementation is hindered by the high cost associated with the parasitic energy consumption during solvent regeneration, along with degradation and corrosion problems. Computer simulations have been widely used to improve our fundamental understanding of CO 2 absorption materials and processes in efforts to design and develop high-performance, cost-effective solvents. Here, we review recent progress in first-principles studies on molecular mechanisms underlying CO 2 absorption into aqueous amines and solvent regeneration. We also briefly discuss aspects that remain unclear, such as degradation and corrosion mechanisms, and the reaction-diffusion behavior of CO 2 at the solvent/gas interface. This review highlights the increasingly significant role of first-principles-based atomistic modeling in exploring the function and properties of candidate materials, as well as the complex physicochemical phenomena underlying CO 2 capture, solvent degradation, and corrosion, especially when direct experimental characterization at the atomic level may be difficult.

The effect of CO2 loading on alkanolamine absorbents in aqueous solutions

“…[1][2][3][4] Complementing engineering studies, computational approaches are essential to reveal the underlying reaction mechanisms of CO 2 absorption and to develop new absorbing compounds. 5,6 Selectivity and reversibility of the absorbent, and its liquid structure properties such as diffusion coefficient and viscosities are important selection criteria. In computational solvent design, molecular dynamics (MD) simulations are able to yield information, which are difficult or sometimes impossible to obtain experimentally.…”

Recent advances in quantum‐mechanical molecular dynamics simulations of proton transfer mechanism in various water‐based environments

“…While novel absorbents have been developed, there has been an increasing interest in developing a rational material design scheme on the basis of the elementary reactions of CO 2 capture in order to further enhance the process performance. The computational studies have made a significant impact on the understanding of the mechanism and the evaluation of the microscopic properties, as observed in the recent comprehensive reviews . In this section, we highlight the success of AIMD simulations in exploring the dynamic process of CO 2 absorption in which PT is an inseparable event.…”

“…The computational studies have made a significant impact on the understanding of the mechanism and the evaluation of the microscopic properties, as observed in the recent comprehensive reviews. [237][238][239] In this section, we highlight the success of AIMD simulations in exploring the dynamic process of CO 2 absorption in which PT is an inseparable event.…”

Effect of Thermal Stabilization on PAN-Derived Electrospun Carbon Nanofibers for CO2 Capture

“…Chemical absorption by aqueous amine-based solvents is a commercially available technology for post-combustion CO 2 capture, but requires a vast amount of equipment and has a high cost due to the high parasitic energy consumption [8,9]. Alternative, more economic adsorption methods are considered very promising, such as those that make use of porous materials including zeolites, MOFs, silica, porous polymers and carbons.…”