Investigating the effect of Cu$^{2+}$ sorption in montmorillonite using density functional theory and molecular dynamics simulations
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arXiv
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| Auteurs principaux: | , , , , , , |
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| Format: | Preprint |
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2023
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| _version_ | 1866909276819161088 |
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| author | Pedram, Yalda Zhang, Yaoting Briggs, Scott Kim, Chang Seok Brochard, Laurent Kalinichev, Andrey G. Béland, Laurent Karim |
| author_facet | Pedram, Yalda Zhang, Yaoting Briggs, Scott Kim, Chang Seok Brochard, Laurent Kalinichev, Andrey G. Béland, Laurent Karim |
| contents | Montmorillonite (MMT) is the main mineral component of bentonite, which is currently proposed as a sealing material in deep geological repositories (DGRs) for used nuclear fuel. In the Canadian program, which will utilize copper-cladded used fuel containers, safety analysis considers the effect of copper corrosion, during which Cu$^{2+}$ ions could potentially be adsorbed by the surrounding MMT. In such a scenario, ion exchange between Na$^+$ and Cu$^{2+}$ is expected. In this study, a multiscale approach that combines electronic density functional theory (DFT) and force-field-based molecular dynamics (MD) simulations was employed to study the effect of introducing Cu$^{2+}$ ions to MMT. An extension to the ClayFF force field is parametrized and validated using DFT to model how Cu$^{2+}$ interacts with clay systems. MD simulations were performed to calculate the interaction free energies between MMT platelets containing Cu$^{2+}$ ions (Cu-MMT) and compared them to inter-platelet interaction energies in Na-MMT and Ca-MMT. Our calculations suggest Cu-MMT develops swelling pressures between those of Ca-MMT and Na-MMT. Furthermore, our MD simulations suggest that Cu$^{2+}$ has MMT interlayer mobility that is significantly slower than that of Ca$^{2+}$. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2311_11139 |
| institution | arXiv |
| publishDate | 2023 |
| record_format | arxiv |
| spellingShingle | Investigating the effect of Cu$^{2+}$ sorption in montmorillonite using density functional theory and molecular dynamics simulations Pedram, Yalda Zhang, Yaoting Briggs, Scott Kim, Chang Seok Brochard, Laurent Kalinichev, Andrey G. Béland, Laurent Karim Materials Science Computational Physics Montmorillonite (MMT) is the main mineral component of bentonite, which is currently proposed as a sealing material in deep geological repositories (DGRs) for used nuclear fuel. In the Canadian program, which will utilize copper-cladded used fuel containers, safety analysis considers the effect of copper corrosion, during which Cu$^{2+}$ ions could potentially be adsorbed by the surrounding MMT. In such a scenario, ion exchange between Na$^+$ and Cu$^{2+}$ is expected. In this study, a multiscale approach that combines electronic density functional theory (DFT) and force-field-based molecular dynamics (MD) simulations was employed to study the effect of introducing Cu$^{2+}$ ions to MMT. An extension to the ClayFF force field is parametrized and validated using DFT to model how Cu$^{2+}$ interacts with clay systems. MD simulations were performed to calculate the interaction free energies between MMT platelets containing Cu$^{2+}$ ions (Cu-MMT) and compared them to inter-platelet interaction energies in Na-MMT and Ca-MMT. Our calculations suggest Cu-MMT develops swelling pressures between those of Ca-MMT and Na-MMT. Furthermore, our MD simulations suggest that Cu$^{2+}$ has MMT interlayer mobility that is significantly slower than that of Ca$^{2+}$. |
| title | Investigating the effect of Cu$^{2+}$ sorption in montmorillonite using density functional theory and molecular dynamics simulations |
| topic | Materials Science Computational Physics |
| url | https://arxiv.org/abs/2311.11139 |