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dc.contributor.authorSilvestri, A.
dc.contributor.authorBudi, A.
dc.contributor.authorAtaman, E.
dc.contributor.authorOlsson, M.
dc.contributor.authorAndersson, M.
dc.contributor.authorStipp, S.
dc.contributor.authorGale, J.
dc.contributor.authorRaiteri, Paolo
dc.date.accessioned2017-11-24T05:25:26Z
dc.date.available2017-11-24T05:25:26Z
dc.date.created2017-11-24T04:48:46Z
dc.date.issued2017
dc.identifier.citationSilvestri, A. and Budi, A. and Ataman, E. and Olsson, M. and Andersson, M. and Stipp, S. and Gale, J. et al. 2017. A quantum mechanically derived force field to predict CO<inf>2</inf>Adsorption on calcite {10.4} in an aqueous environment. Journal of Physical Chemistry C. 121 (39).
dc.identifier.urihttp://hdl.handle.net/20.500.11937/58390
dc.identifier.doi10.1021/acs.jpcc.7b06700
dc.description.abstract

© 2017 American Chemical Society. Density functional theory (DFT) with semiempirical dispersion corrections (DFT-D2) has been used to calculate the binding energy of a CO 2 molecule on the calcite {10.4} surface for different positions and orientations. This generated potential energy landscape was then used to parametrize a classical force field. From this, we used metadynamics (MTD) to derive free energy profiles at 300 and 350 K for CO 2 binding to calcite, CO 2 binding with Ca 2+ , and pairing of two CO 2 molecules, all for aqueous conditions. We subsequently performed classical molecular dynamics (MD) simulations of CO 2 and water on the {10.4} surface at pressures and temperatures relevant for CO 2 geological storage. Density profiles show characteristic structured water layering at the calcite surface and two distinct phases of water and CO 2 . We have also calculated the densities of the CO 2 -rich and water-rich phases and thereby determined the mutual solubilities. For all the pressures and temperatures in the studied range, CO 2 was unable to penetrate the ordered water layers and adsorb directly on the solid surface. This is further confirmed by the free energy profiles showing that in the presence of water there is neither direct adsorption to the {10.4} surface nor contact binding of CO 2 with Ca 2+ . Rather, we saw a weak affinity for the surface of the ordered water layers. At 5 MPa and 323 K, we observed the nucleation of a CO 2 droplet located above two structured water layers over the solid. It could not penetrate the structured water but remained bound to the second water layer for the first 10 ns of the simulation before eventually detaching and diffusing away.

dc.publisherAmerican Chemical Society
dc.titleA quantum mechanically derived force field to predict CO<inf>2</inf>Adsorption on calcite {10.4} in an aqueous environment
dc.typeJournal Article
dcterms.source.volume121
dcterms.source.number39
dcterms.source.issn1932-7447
dcterms.source.titleJournal of Physical Chemistry C
curtin.departmentDepartment of Chemistry
curtin.accessStatusFulltext not available


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