Atomistic modeling of CO2 capture in primary and tertiary amines – Heat of absorption and density changes

With the aim of exploring new amine-based chemistry for CO2 capture at large industrial scales we performed atomistic modeling of CO2 chemisorption in aqueous solutions of primary and tertiary amines. DFT-based quantum chemical solvation calculations are shown to yield a number of important results, including the relative stability of ion species (carbamate vs. bicarbonate), heat of absorption, and density and volume changes as a function of CO2 loading. Good agreement of simulation results with available experimental data provides confidence in the accuracy of such computational methods in predicting properties of new solvent systems and capture designs.