Location of Artinite (Mg2CO3(OH)2·3H2O) within the MgO-CO2-H2O System using Ab initio Thermodynamics

Joshua S. Tse, James Grant, Jonathan M. Skelton, Lisa J. Gillie, Runliang Zhu, Giovanni L. Pesce, Richard J. Ball, Stephen C. Parker, Marco Molinari

Research output: Contribution to journalArticlepeer-review

Abstract

The MgO-CO2-H2O system has a variety of important industrial applications including catalysis, immobilisation of radionuclides and heavy metals, construction, and mineralisation and permanent storage of anthropogenic CO2. Here, we examine a computational approach to generate phase stability plots of the MgO-CO2-H2O system that do not rely on traditional experimental corrections for the solid phases. We compare the predictions made by several dispersion-corrected density-functional theory schemes, and we include the temperature-dependent Gibbs free energy through the quasiharmonic approximation. We locate the Artinite phase (Mg2CO3(OH)2·3H2O) within the MgO-CO2-H2O phase stability plot, and we demonstrate that this widely-overlooked hydrated and carbonated phase is metastable and can be stabilised by inhibiting the formation of fully-carbonated stable phases. This may apply broadly to other lesser known phases. These findings provide new data to explain conflicting results from experimental studies, and demonstrate how this phase can potentially be stabilised by optimising the synthesis conditions.
Original languageEnglish
JournalPhysical Chemistry Chemical Physics
Publication statusAccepted/In press - 15 Jun 2023

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