Ion Sieving in Two-Dimensional Membranes from First Principles
Fuente:
arXiv
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| Autori principali: | , |
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| Natura: | Preprint |
| Pubblicazione: |
2024
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| _version_ | 1866909433044402176 |
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| author | Bonnet, Nicéphore Marzari, Nicola |
| author_facet | Bonnet, Nicéphore Marzari, Nicola |
| contents | A first-principles approach for calculating ion separation in solution through two-dimensional (2D) membranes is proposed and applied. Ionic energy profiles across the membrane are obtained first, where solvation effects are simulated explicitly with machine-learning molecular dynamics, electrostatic corrections are applied to remove finite-size capacitive effects, and a mean-field treatment of the charging of the electrochemical double layer is used. Entropic contributions are assessed analytically and validated against thermodynamic integration. Ionic separations are then inferred through a microkinetic model of the filtration process, accounting for steady-state charge separation effects across the membrane. The approach is applied to Li$^{+}$, Na$^{+}$, K$^{+}$ sieving through a crown-ether functionalized graphene membrane, with a case study of the mechanisms for a highly selective and efficient extraction of lithium from aqueous solutions. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2412_13899 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Ion Sieving in Two-Dimensional Membranes from First Principles Bonnet, Nicéphore Marzari, Nicola Soft Condensed Matter Materials Science A first-principles approach for calculating ion separation in solution through two-dimensional (2D) membranes is proposed and applied. Ionic energy profiles across the membrane are obtained first, where solvation effects are simulated explicitly with machine-learning molecular dynamics, electrostatic corrections are applied to remove finite-size capacitive effects, and a mean-field treatment of the charging of the electrochemical double layer is used. Entropic contributions are assessed analytically and validated against thermodynamic integration. Ionic separations are then inferred through a microkinetic model of the filtration process, accounting for steady-state charge separation effects across the membrane. The approach is applied to Li$^{+}$, Na$^{+}$, K$^{+}$ sieving through a crown-ether functionalized graphene membrane, with a case study of the mechanisms for a highly selective and efficient extraction of lithium from aqueous solutions. |
| title | Ion Sieving in Two-Dimensional Membranes from First Principles |
| topic | Soft Condensed Matter Materials Science |
| url | https://arxiv.org/abs/2412.13899 |