The main contribution to the mechanistic studies of CO 2 binding in amines comes from electronic structure calculations of isolated clusters. These earlier works pointed out the charge transfer involved in the formation of the zwitterion intermediate and proton transfer required to produce the most stable carbamate and carbamic acid species. These electronic structure calculations also provided insights into the effect of the amine chemical composition and presence of water into the adsorption energy of CO 2 on the amine. Despite their relevance to the field, very little is known about the temperature and solvation effects on the mechanism and thermodynamics of CO 2 binding in condensed phase amines.