Location of Artinite (Mg2CO3(OH)2.3H2O) within the MgO–CO2–H2O system using ab initio thermodynamics

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

doi:10.1039/d3cp00518f

Location of Artinite (Mg2CO3(OH)2.3H2O) within the MgO–CO2–H2O system using ab initio thermodynamics

Joshua 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 journal › Article › peer-review

2 Citations (SciVal)

Abstract

The MgO-CO ₂-H ₂O system have a variety of important industrial applications including in catalysis, immobilisation of radionuclides and heavy metals, construction, and mineralisation and permanent storage of anthropogenic CO ₂. Here, we develop a computational approach to generate phase stability plots for the MgO-CO ₂-H ₂O 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 quasi-harmonic approximation. We locate the Artinite phase (Mg ₂CO ₃(OH) ₂·3H ₂O) within the MgO-CO ₂-H ₂O 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. Similar considerations may apply more broadly to other lesser known phases. These findings provide new insight to explain conflicting results from experimental studies, and demonstrate how this phase can potentially be stabilised by optimising the synthesis conditions.

Original language	English
Pages (from-to)	18011-18022
Number of pages	12
Journal	Physical chemistry chemical physics : PCCP
Volume	25
Issue number	27
Early online date	15 Jun 2023
DOIs	https://doi.org/10.1039/d3cp00518f
Publication status	Published - 21 Jul 2023

Bibliographical note

Acknowledgements:
The authors would like to thank the UK Engineering and Physical Sciences Research Council (EPSRC; EP/K025597/1 and EP/R010366/1), the Royal Society (Newton Advanced Fellowship NA150190), UK Research and Innovation (UKRI; MR/T043121/1), and the Collaborative Computational Project 5 (CCP5), which is funded by the EPSRC (EP/J010480/1), for financial support. The computational work made use of the UK national HPC service, ARCHER/ARCHER2, via the Materials Chemistry Consortium (MCC), which is funded by the EPSRC (EP/L000202/1, EP/R029431/1 and EP/X035859/1). We also made use of the Balena HPC (University of Bath), and the Orion computing facility and the Violeta HPC (University of Huddersfield).

Data availability:
Raw data are available from https://doi.org/10.17632/s96szk84zb.1

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10.1039/d3cp00518fLicence: CC BY

Cite this

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title = "Location of Artinite (Mg2CO3(OH)2.3H2O) within the MgO–CO2–H2O system using ab initio thermodynamics",

abstract = "The MgO-CO 2-H 2O system have a variety of important industrial applications including in catalysis, immobilisation of radionuclides and heavy metals, construction, and mineralisation and permanent storage of anthropogenic CO 2. Here, we develop a computational approach to generate phase stability plots for the MgO-CO 2-H 2O 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 quasi-harmonic approximation. We locate the Artinite phase (Mg 2CO 3(OH) 2·3H 2O) within the MgO-CO 2-H 2O 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. Similar considerations may apply more broadly to other lesser known phases. These findings provide new insight to explain conflicting results from experimental studies, and demonstrate how this phase can potentially be stabilised by optimising the synthesis conditions.",

author = "Joshua Tse and James Grant and Skelton, {Jonathan M.} and Gillie, {Lisa J.} and Runliang Zhu and Pesce, {Giovanni L.} and Ball, {Richard J.} and Parker, {Stephen C.} and Marco Molinari",

note = "Acknowledgements: The authors would like to thank the UK Engineering and Physical Sciences Research Council (EPSRC; EP/K025597/1 and EP/R010366/1), the Royal Society (Newton Advanced Fellowship NA150190), UK Research and Innovation (UKRI; MR/T043121/1), and the Collaborative Computational Project 5 (CCP5), which is funded by the EPSRC (EP/J010480/1), for financial support. The computational work made use of the UK national HPC service, ARCHER/ARCHER2, via the Materials Chemistry Consortium (MCC), which is funded by the EPSRC (EP/L000202/1, EP/R029431/1 and EP/X035859/1). We also made use of the Balena HPC (University of Bath), and the Orion computing facility and the Violeta HPC (University of Huddersfield). Data availability: Raw data are available from https://doi.org/10.17632/s96szk84zb.1",

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doi = "10.1039/d3cp00518f",

language = "English",

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AU - Tse, Joshua

AU - Grant, James

AU - Skelton, Jonathan M.

AU - Gillie, Lisa J.

AU - Zhu, Runliang

AU - Pesce, Giovanni L.

AU - Ball, Richard J.

AU - Parker, Stephen C.

AU - Molinari, Marco

N1 - Acknowledgements: The authors would like to thank the UK Engineering and Physical Sciences Research Council (EPSRC; EP/K025597/1 and EP/R010366/1), the Royal Society (Newton Advanced Fellowship NA150190), UK Research and Innovation (UKRI; MR/T043121/1), and the Collaborative Computational Project 5 (CCP5), which is funded by the EPSRC (EP/J010480/1), for financial support. The computational work made use of the UK national HPC service, ARCHER/ARCHER2, via the Materials Chemistry Consortium (MCC), which is funded by the EPSRC (EP/L000202/1, EP/R029431/1 and EP/X035859/1). We also made use of the Balena HPC (University of Bath), and the Orion computing facility and the Violeta HPC (University of Huddersfield). Data availability: Raw data are available from https://doi.org/10.17632/s96szk84zb.1

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N2 - The MgO-CO 2-H 2O system have a variety of important industrial applications including in catalysis, immobilisation of radionuclides and heavy metals, construction, and mineralisation and permanent storage of anthropogenic CO 2. Here, we develop a computational approach to generate phase stability plots for the MgO-CO 2-H 2O 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 quasi-harmonic approximation. We locate the Artinite phase (Mg 2CO 3(OH) 2·3H 2O) within the MgO-CO 2-H 2O 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. Similar considerations may apply more broadly to other lesser known phases. These findings provide new insight to explain conflicting results from experimental studies, and demonstrate how this phase can potentially be stabilised by optimising the synthesis conditions.

AB - The MgO-CO 2-H 2O system have a variety of important industrial applications including in catalysis, immobilisation of radionuclides and heavy metals, construction, and mineralisation and permanent storage of anthropogenic CO 2. Here, we develop a computational approach to generate phase stability plots for the MgO-CO 2-H 2O 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 quasi-harmonic approximation. We locate the Artinite phase (Mg 2CO 3(OH) 2·3H 2O) within the MgO-CO 2-H 2O 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. Similar considerations may apply more broadly to other lesser known phases. These findings provide new insight to explain conflicting results from experimental studies, and demonstrate how this phase can potentially be stabilised by optimising the synthesis conditions.

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DO - 10.1039/d3cp00518f

M3 - Article

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JO - Physical chemistry chemical physics : PCCP

JF - Physical chemistry chemical physics : PCCP

IS - 27

ER -

Location of Artinite (Mg2CO3(OH)2.3H2O) within the MgO–CO2–H2O system using ab initio thermodynamics

Abstract

Bibliographical note

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Experimentally Verfied Atomistic Modelling of Lime in Construction Materials

CCP5 The Computer Simulation of Condensed Phases

Cite this

Location of Artinite (Mg2CO3(OH)2.3H2O) within the MgO–CO2–H2O system using ab initio thermodynamics

Abstract

Bibliographical note

Access to Document

Other files and links

Fingerprint

Projects

Experimentally Verfied Atomistic Modelling of Lime in Construction Materials

CCP5 The Computer Simulation of Condensed Phases

Cite this