Structure, dynamics and stability of water/scCO2/mineral interfaces from ab initio molecular dynamics simulations

Mal Soon Lee, B. Peter McGrail, Roger Rousseau, Vassiliki Alexandra Glezakou

Research output: Contribution to journalArticle

13 Citations (Scopus)

Abstract

The boundary layer at solid-liquid interfaces is a unique reaction environment that poses significant scientific challenges to characterize and understand by experimentation alone. Using ab initio molecular dynamics (AIMD) methods, we report on the structure and dynamics of boundary layer formation, cation mobilization and carbonation under geologic carbon sequestration scenarios (T = 323 K and P = 90 bar) on a prototypical anorthite (001) surface. At low coverage, water film formation is enthalpically favored, but entropically hindered. Simulated adsorption isotherms show that a water monolayer will form even at the low water concentrations of water-saturated scCO2. Carbonation reactions readily occur at electron-rich terminal Oxygen sites adjacent to cation vacancies that readily form in the presence of a water monolayer. These results point to a carbonation mechanism that does not require prior carbonic acid formation in the bulk liquid. This work also highlights the modern capabilities of theoretical methods to address structure and reactivity at interfaces of high chemical complexity.

Original languageEnglish
Article number14857
JournalScientific Reports
Volume5
DOIs
Publication statusPublished - Oct 12 2015

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simulation
water
boundary layer
cation
liquid
anorthite
carbon sequestration
mobilization
isotherm
mineral water
adsorption
electron
oxygen
acid
method
chemical

ASJC Scopus subject areas

  • General

Cite this

Structure, dynamics and stability of water/scCO2/mineral interfaces from ab initio molecular dynamics simulations. / Lee, Mal Soon; Peter McGrail, B.; Rousseau, Roger; Glezakou, Vassiliki Alexandra.

In: Scientific Reports, Vol. 5, 14857, 12.10.2015.

Research output: Contribution to journalArticle

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