Computational Insights into Mg2+ Dehydration in the Presence of Carbonate

Water exchange around a free magnesium ion and magnesium paired with carbonate in aqueous solution was studied using free energy methods. Both a rigid-ion and a polarizable force field based on the AMOEBA model were examined. The parameters were adjusted to accurately reproduce the hydration structu...

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Main Authors: Aufort, Julie, Raiteri, Paolo, Gale, Julian
Format: Journal Article
Language:English
Published: AMER CHEMICAL SOC 2022
Subjects:
Online Access:http://purl.org/au-research/grants/arc/FL180100087
http://hdl.handle.net/20.500.11937/91505
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author Aufort, Julie
Raiteri, Paolo
Gale, Julian
author_facet Aufort, Julie
Raiteri, Paolo
Gale, Julian
author_sort Aufort, Julie
building Curtin Institutional Repository
collection Online Access
description Water exchange around a free magnesium ion and magnesium paired with carbonate in aqueous solution was studied using free energy methods. Both a rigid-ion and a polarizable force field based on the AMOEBA model were examined. The parameters were adjusted to accurately reproduce the hydration structures of magnesium and carbonate in aqueous solution. The magnesium carbonate ion pairing free energies calculated with both force fields were found to be in excellent agreement with experimental data. Metadynamics simulations of the water exchange conducted with both models revealed that the formation of a contact magnesium carbonate ion pair significantly decreases the energy barrier for water exchange relative to the free magnesium ion in solution. This finding suggests that the presence of carbonate could accelerate the water exchange around magnesium and constitutes a first step toward a better understanding of the atomic-scale mechanisms involved in the nucleation of magnesium-bearing carbonate minerals.
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spelling curtin-20.500.11937-915052023-05-10T07:38:43Z Computational Insights into Mg2+ Dehydration in the Presence of Carbonate Aufort, Julie Raiteri, Paolo Gale, Julian Science & Technology Physical Sciences Chemistry, Multidisciplinary Geochemistry & Geophysics Chemistry Molecular dynamics Water exchange Free energy Polarization MOLECULAR-DYNAMICS SIMULATIONS GIBBS FREE-ENERGY WATER EXCHANGE DOLOMITE PRECIPITATION DIFFUSION-COEFFICIENTS ION HYDRATION THERMODYNAMICS SOLVATION PARAMETERS MECHANISM Water exchange around a free magnesium ion and magnesium paired with carbonate in aqueous solution was studied using free energy methods. Both a rigid-ion and a polarizable force field based on the AMOEBA model were examined. The parameters were adjusted to accurately reproduce the hydration structures of magnesium and carbonate in aqueous solution. The magnesium carbonate ion pairing free energies calculated with both force fields were found to be in excellent agreement with experimental data. Metadynamics simulations of the water exchange conducted with both models revealed that the formation of a contact magnesium carbonate ion pair significantly decreases the energy barrier for water exchange relative to the free magnesium ion in solution. This finding suggests that the presence of carbonate could accelerate the water exchange around magnesium and constitutes a first step toward a better understanding of the atomic-scale mechanisms involved in the nucleation of magnesium-bearing carbonate minerals. 2022 Journal Article http://hdl.handle.net/20.500.11937/91505 10.1021/acsearthspacechem.1c00389 English http://purl.org/au-research/grants/arc/FL180100087 AMER CHEMICAL SOC fulltext
spellingShingle Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Geochemistry & Geophysics
Chemistry
Molecular dynamics
Water exchange
Free energy
Polarization
MOLECULAR-DYNAMICS SIMULATIONS
GIBBS FREE-ENERGY
WATER EXCHANGE
DOLOMITE PRECIPITATION
DIFFUSION-COEFFICIENTS
ION HYDRATION
THERMODYNAMICS
SOLVATION
PARAMETERS
MECHANISM
Aufort, Julie
Raiteri, Paolo
Gale, Julian
Computational Insights into Mg2+ Dehydration in the Presence of Carbonate
title Computational Insights into Mg2+ Dehydration in the Presence of Carbonate
title_full Computational Insights into Mg2+ Dehydration in the Presence of Carbonate
title_fullStr Computational Insights into Mg2+ Dehydration in the Presence of Carbonate
title_full_unstemmed Computational Insights into Mg2+ Dehydration in the Presence of Carbonate
title_short Computational Insights into Mg2+ Dehydration in the Presence of Carbonate
title_sort computational insights into mg2+ dehydration in the presence of carbonate
topic Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Geochemistry & Geophysics
Chemistry
Molecular dynamics
Water exchange
Free energy
Polarization
MOLECULAR-DYNAMICS SIMULATIONS
GIBBS FREE-ENERGY
WATER EXCHANGE
DOLOMITE PRECIPITATION
DIFFUSION-COEFFICIENTS
ION HYDRATION
THERMODYNAMICS
SOLVATION
PARAMETERS
MECHANISM
url http://purl.org/au-research/grants/arc/FL180100087
http://hdl.handle.net/20.500.11937/91505