Structure, dynamics and stability of water/scCO2/mineral interfaces from ab initio molecular dynamics simulations
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,...
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ftpubmed:oai:pubmedcentral.nih.gov:4600984 2023-05-15T15:52:40+02:00 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 2015-10-12 http://www.ncbi.nlm.nih.gov/pmc/articles/PMC4600984/ http://www.ncbi.nlm.nih.gov/pubmed/26456362 https://doi.org/10.1038/srep14857 en eng Nature Publishing Group http://www.ncbi.nlm.nih.gov/pmc/articles/PMC4600984/ http://www.ncbi.nlm.nih.gov/pubmed/26456362 http://dx.doi.org/10.1038/srep14857 Copyright © 2015, Macmillan Publishers Limited http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ CC-BY Article Text 2015 ftpubmed https://doi.org/10.1038/srep14857 2015-10-25T00:16:55Z 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. Text Carbonic acid PubMed Central (PMC) Scientific Reports 5 1 |
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Article Lee, Mal-Soon Peter McGrail, B. Rousseau, Roger Glezakou, Vassiliki-Alexandra Structure, dynamics and stability of water/scCO2/mineral interfaces from ab initio molecular dynamics simulations |
topic_facet |
Article |
description |
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. |
format |
Text |
author |
Lee, Mal-Soon Peter McGrail, B. Rousseau, Roger Glezakou, Vassiliki-Alexandra |
author_facet |
Lee, Mal-Soon Peter McGrail, B. Rousseau, Roger Glezakou, Vassiliki-Alexandra |
author_sort |
Lee, Mal-Soon |
title |
Structure, dynamics and stability of water/scCO2/mineral interfaces from ab initio molecular dynamics simulations |
title_short |
Structure, dynamics and stability of water/scCO2/mineral interfaces from ab initio molecular dynamics simulations |
title_full |
Structure, dynamics and stability of water/scCO2/mineral interfaces from ab initio molecular dynamics simulations |
title_fullStr |
Structure, dynamics and stability of water/scCO2/mineral interfaces from ab initio molecular dynamics simulations |
title_full_unstemmed |
Structure, dynamics and stability of water/scCO2/mineral interfaces from ab initio molecular dynamics simulations |
title_sort |
structure, dynamics and stability of water/scco2/mineral interfaces from ab initio molecular dynamics simulations |
publisher |
Nature Publishing Group |
publishDate |
2015 |
url |
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC4600984/ http://www.ncbi.nlm.nih.gov/pubmed/26456362 https://doi.org/10.1038/srep14857 |
genre |
Carbonic acid |
genre_facet |
Carbonic acid |
op_relation |
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC4600984/ http://www.ncbi.nlm.nih.gov/pubmed/26456362 http://dx.doi.org/10.1038/srep14857 |
op_rights |
Copyright © 2015, Macmillan Publishers Limited http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ |
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CC-BY |
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https://doi.org/10.1038/srep14857 |
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Scientific Reports |
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