title: Transport Properties of Amine/Carbon Dioxide Reactive Mixtures and Implications to Carbon Capture Technologies.
abstract: The structure and transport properties of physisorbed and chemisorbed CO2 in model polyamine liquids (hexamethylenediamine and diethylenetriamine) are studied via molecular dynamics simulations. Such systems are relevant to CO2 absorption processes where nonaqueous amines are used as absorbents (e.g., when impregnated or grafted onto mesoporous media or misted in the gas phase). It is shown that accounting for the ionic speciation resulting from CO2 chemisorption enabled us to capture the qualitative changes in extent of absorption and fluidity with time that are observed in thermogravimetric experiments. Simulations reveal that high enough concentration of reacted CO2 leads to strong intermolecular ionic interactions and the arrest of molecular translations. The transport properties obtained from the simulations of the ionic speciated mixtures are also used to construct an approximate continuum-level model for the CO2 absorption process that mimics thermogravimetric experiments.
authors.affiliation: †School of Chemical and Biomolecular Engineering, Cornell University, Ithaca New York 14853, United States.
authors.forename: Salomon
authors.initials: S
authors.lastname: Turgman-Cohen
authors.forename: Emmanuel P
authors.initials: EP
authors.lastname: Giannelis
authors.affiliation: †School of Chemical and Biomolecular Engineering, Cornell University, Ithaca New York 14853, United States.
authors.forename: Fernando A
authors.initials: FA
authors.lastname: Escobedo
keywords: capture; carbon dioxide; molecular dynamics; multiscale; polyamines; sequestration