Diffusion in CaCO3 Calcite Investigated ...
Document type :
Article dans une revue scientifique
DOI :
Permalink :
Title :
Diffusion in CaCO3 Calcite Investigated by Atomic-Scale Simulations
Author(s) :
Besson, Rémy [Auteur]
Unité Matériaux et Transformations - UMR 8207 [UMET]
Tingaud, David [Auteur]
Laboratoire des Sciences des Procédés et des Matériaux [LSPM]
Favergeon, Loïc [Auteur]
Laboratoire Georges Friedel [LGF-ENSMSE]
Unité Matériaux et Transformations - UMR 8207 [UMET]
Tingaud, David [Auteur]
Laboratoire des Sciences des Procédés et des Matériaux [LSPM]
Favergeon, Loïc [Auteur]
Laboratoire Georges Friedel [LGF-ENSMSE]
Journal title :
The Journal of Physical Chemistry C
Abbreviated title :
J. Phys. Chem. C
Volume number :
123
Pages :
21825-21837
Publisher :
American Chemical Society (ACS)
Publication date :
2019-08-14
English keyword(s) :
atomic-scale
calcite
atomic diffusion
carbonation
calcite
atomic diffusion
carbonation
HAL domain(s) :
Chimie/Matériaux
Physique [physics]/Matière Condensée [cond-mat]/Science des matériaux [cond-mat.mtrl-sci]
Physique [physics]/Matière Condensée [cond-mat]/Science des matériaux [cond-mat.mtrl-sci]
English abstract : [en]
In the context of CO2 storage, we used ab initio-based atomic-scale modelings and simulations to study oxygen and carbon diffusion in CaCO3 calcite. In overall agreement with earlier experimental findings, oxygen diffusion ...
Show more >In the context of CO2 storage, we used ab initio-based atomic-scale modelings and simulations to study oxygen and carbon diffusion in CaCO3 calcite. In overall agreement with earlier experimental findings, oxygen diffusion is found to take place possibly by either interstitial or vacancy mechanisms depending on the thermodynamic conditions. Contrary to almost isotropic interstitial diffusion, the vacancy mechanism strongly favors oxygen jumps within (111) planes characteristic of the CaCO3 layered structure, with significant less-than-unity correlation factors. Our simulations show that such mechanisms cannot be applied to carbon, and complex point defects may be required to explain the diffusion of this element. While stability arguments indicate that vacancy complexes formed with CO or CO3 missing groups may be efficient candidates to convey C diffusion, no low-energy migration path could be identified for these complexes. Focusing on the mostly stable CO vacancy complex and using generic values for unknown migration energies, kinetic Monte Carlo simulations show that this complex mechanism may be responsible for C diffusion roughly 2 orders of magnitude above its oxygen counterpart.Show less >
Show more >In the context of CO2 storage, we used ab initio-based atomic-scale modelings and simulations to study oxygen and carbon diffusion in CaCO3 calcite. In overall agreement with earlier experimental findings, oxygen diffusion is found to take place possibly by either interstitial or vacancy mechanisms depending on the thermodynamic conditions. Contrary to almost isotropic interstitial diffusion, the vacancy mechanism strongly favors oxygen jumps within (111) planes characteristic of the CaCO3 layered structure, with significant less-than-unity correlation factors. Our simulations show that such mechanisms cannot be applied to carbon, and complex point defects may be required to explain the diffusion of this element. While stability arguments indicate that vacancy complexes formed with CO or CO3 missing groups may be efficient candidates to convey C diffusion, no low-energy migration path could be identified for these complexes. Focusing on the mostly stable CO vacancy complex and using generic values for unknown migration energies, kinetic Monte Carlo simulations show that this complex mechanism may be responsible for C diffusion roughly 2 orders of magnitude above its oxygen counterpart.Show less >
Language :
Anglais
Peer reviewed article :
Oui
Audience :
Internationale
Popular science :
Non
Administrative institution(s) :
Université de Lille
CNRS
INRA
ENSCL
CNRS
INRA
ENSCL
Collections :
Research team(s) :
Métallurgie Physique et Génie des Matériaux
Submission date :
2020-12-03T09:01:49Z
2020-12-07T10:59:42Z
2021-02-09T08:44:00Z
2020-12-07T10:59:42Z
2021-02-09T08:44:00Z
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