Nanoconfinement matters in humidified CO 2 interaction with metal silicates
With enigmatic observations of enhanced reactivity of wet CO 2 -rich fluids with metal silicates, the mechanistic understanding of molecular processes governing carbonation proves critical in designing secure geological carbon sequestration and economical carbonated concrete technologies. Here, we u...
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ftosti:oai:osti.gov:1893846 2023-07-30T04:02:55+02:00 Nanoconfinement matters in humidified CO 2 interaction with metal silicates Zare, Siavash Uddin, K. M. Salah Funk, Andreas Miller, Quin S. Abdolhosseini Qomi, Mohammad Javad 2022-11-15 application/pdf http://www.osti.gov/servlets/purl/1893846 https://www.osti.gov/biblio/1893846 https://doi.org/10.1039/d2en00148a unknown http://www.osti.gov/servlets/purl/1893846 https://www.osti.gov/biblio/1893846 https://doi.org/10.1039/d2en00148a doi:10.1039/d2en00148a 54 ENVIRONMENTAL SCIENCES 2022 ftosti https://doi.org/10.1039/d2en00148a 2023-07-11T10:15:44Z With enigmatic observations of enhanced reactivity of wet CO 2 -rich fluids with metal silicates, the mechanistic understanding of molecular processes governing carbonation proves critical in designing secure geological carbon sequestration and economical carbonated concrete technologies. Here, we use the first principle and classical molecular simulations to probe the impact of nanoconfinement on physicochemical processes at the rock–water–CO 2 interface. We choose nanoporous calcium–silicate–hydrate (C–S–H) and forsterite (Mg 2 SiO 4 ) as model metal silicate surfaces that are of significance in cement chemistry and geochemistry communities, respectively. We show that while a nanometer-thick interfacial water film persists at unsaturated conditions consistent with in situ infrared spectroscopy, the phase behavior of the water–CO 2 mixture changes from its bulk counterpart depending on the surface chemistry and nanoconfinement. We also observe enhanced solubility at the interface of water and CO 2 phases, which could amplify the CO 2 speciation rate. Additionally, through free energy calculations, we show that CO 2 could be found in a metastable state near the C–S–H surface, which can potentially react with surface water and hydroxyl groups to form carbonic acid and bicarbonate. These findings support the explicit consideration of nanoconfinement effects in reactive and non-reactive pore-scale processes. Other/Unknown Material Carbonic acid SciTec Connect (Office of Scientific and Technical Information - OSTI, U.S. Department of Energy) Environmental Science: Nano 9 10 3766 3779 |
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SciTec Connect (Office of Scientific and Technical Information - OSTI, U.S. Department of Energy) |
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54 ENVIRONMENTAL SCIENCES |
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54 ENVIRONMENTAL SCIENCES Zare, Siavash Uddin, K. M. Salah Funk, Andreas Miller, Quin S. Abdolhosseini Qomi, Mohammad Javad Nanoconfinement matters in humidified CO 2 interaction with metal silicates |
topic_facet |
54 ENVIRONMENTAL SCIENCES |
description |
With enigmatic observations of enhanced reactivity of wet CO 2 -rich fluids with metal silicates, the mechanistic understanding of molecular processes governing carbonation proves critical in designing secure geological carbon sequestration and economical carbonated concrete technologies. Here, we use the first principle and classical molecular simulations to probe the impact of nanoconfinement on physicochemical processes at the rock–water–CO 2 interface. We choose nanoporous calcium–silicate–hydrate (C–S–H) and forsterite (Mg 2 SiO 4 ) as model metal silicate surfaces that are of significance in cement chemistry and geochemistry communities, respectively. We show that while a nanometer-thick interfacial water film persists at unsaturated conditions consistent with in situ infrared spectroscopy, the phase behavior of the water–CO 2 mixture changes from its bulk counterpart depending on the surface chemistry and nanoconfinement. We also observe enhanced solubility at the interface of water and CO 2 phases, which could amplify the CO 2 speciation rate. Additionally, through free energy calculations, we show that CO 2 could be found in a metastable state near the C–S–H surface, which can potentially react with surface water and hydroxyl groups to form carbonic acid and bicarbonate. These findings support the explicit consideration of nanoconfinement effects in reactive and non-reactive pore-scale processes. |
author |
Zare, Siavash Uddin, K. M. Salah Funk, Andreas Miller, Quin S. Abdolhosseini Qomi, Mohammad Javad |
author_facet |
Zare, Siavash Uddin, K. M. Salah Funk, Andreas Miller, Quin S. Abdolhosseini Qomi, Mohammad Javad |
author_sort |
Zare, Siavash |
title |
Nanoconfinement matters in humidified CO 2 interaction with metal silicates |
title_short |
Nanoconfinement matters in humidified CO 2 interaction with metal silicates |
title_full |
Nanoconfinement matters in humidified CO 2 interaction with metal silicates |
title_fullStr |
Nanoconfinement matters in humidified CO 2 interaction with metal silicates |
title_full_unstemmed |
Nanoconfinement matters in humidified CO 2 interaction with metal silicates |
title_sort |
nanoconfinement matters in humidified co 2 interaction with metal silicates |
publishDate |
2022 |
url |
http://www.osti.gov/servlets/purl/1893846 https://www.osti.gov/biblio/1893846 https://doi.org/10.1039/d2en00148a |
genre |
Carbonic acid |
genre_facet |
Carbonic acid |
op_relation |
http://www.osti.gov/servlets/purl/1893846 https://www.osti.gov/biblio/1893846 https://doi.org/10.1039/d2en00148a doi:10.1039/d2en00148a |
op_doi |
https://doi.org/10.1039/d2en00148a |
container_title |
Environmental Science: Nano |
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9 |
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10 |
container_start_page |
3766 |
op_container_end_page |
3779 |
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1772813813193637888 |