Classical Polarizable Force Field to Study Hydrated Hectorite: Optimization on DFT Calculations and Validation against XRD Data
Abstract
:1. Introduction
2. Parametrization of PIM Force Field
2.1. Characteristics of the Polarizable Ion Model
2.2. Optimization Procedure
- Generation of a series of representative configurations using classical molecular dynamics (MD)
- DFT calculations on each of these configurations
- Minimization of the error function on the dipoles with respect to the parameters of the polarization term (V) and of with respect to the repulsion term (V):
2.3. Simulation Details
2.3.1. Dry Hectorites
2.3.2. Hydrated Na-Hectorite
2.4. Force Field Parameters
3. Validation of the Force Field
3.1. Simulations Details
3.2. XRD Materials and Methods
3.3. Results and Discussion
3.3.1. Dry Hectorites
3.3.2. Hydrated Hectorites
3.4. Beyond Validation: Dynamics
4. Conclusions
Supplementary Materials
Author Contributions
Acknowledgments
Conflicts of Interest
References
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(Å) | (Å) | Angle () | (kcal/mol) | (Å) | (Å) | |
---|---|---|---|---|---|---|
0.9752 | 0.215 | 104.52 | 0.1825 | 3.2340 | 0.5190 | 1.444 |
Systems | ||
---|---|---|
Dry hectorite | 0.123 | 0.561 |
Wet hectorite | 0.170 | 3.025 |
Damping Interaction between and | |||||||
---|---|---|---|---|---|---|---|
Ion Pair (ij) | (Ha) | (Å−1) | (Ha·Å6) | (Ha·Å8) | (Å−1) | (Å−1) | |
Li-O | 9.68 | 2.78 | 0.0477 | 0.156 | 4.17 | 1.19 | 2.79 |
Li-O | 24.6 | 3.82 | 0.0477 | 0.156 | 4.17 | 1.16 | 2.78 |
Li-OW | 0.427 | 3.50 | 0.0477 | 0.156 | 4.17 | - | - |
Li-MW | - | - | - | - | - | 3.75 | 1.24 |
Li-Na | - | - | - | - | - | 0.587 | 4.64 |
Li-Cs | - | - | - | - | - | 0.0423 | 4.99 |
Li-Ca | - | - | - | - | - | 3.87 | 3.64 |
Li-Sr | - | - | - | - | - | 0.895 | 4.69 |
System | Super Cell Dimensions | A (Å) | B (Å) | h (Å) | Number of HO per Unit Cell |
---|---|---|---|---|---|
monohydrated (1W) | 5 × 2 × 2 | 26.3 | 18.2 | 12.53 | 4.2 |
bihydrated (2W) | 5 × 2 × 2 | 26.3 | 18.2 | 15.51 | 8.9 |
Counterion | a (Å) | b (Å) | c (Å) | h (Å) | (deg) | (deg) | (deg) |
---|---|---|---|---|---|---|---|
Na | 5.235 (1) | 9.108 (4) | 9.813 (7) | 9.711 (1) | 91.8 (2) | 96.4 (2) | 90.02 (5) |
Cs | 5.258 (5) | 9.106 (7) | 10.674 (7) | 10.524 (5) | 89.90 (6) | 99.53 (7) | 89.95 (4) |
Ca | 5.255 (9) | 9.15 (2) | 10.23 (1) | 9.676 (1) | 90.1 (1) | 108.1 (2) | 90.2 (1) |
Sr | 5.231 (6) | 9.11 (2) | 10.28 (2) | 9.767 (5) | 90.1 (2) | 106.9 (2) | 90.1 (1) |
talc (exp) [87] | 5.293 | 9.179 | 9.469 | 9.381 | 90.57 | 98.91 | 90.03 |
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Hånde, R.; Ramothe, V.; Tesson, S.; Dazas, B.; Ferrage, E.; Lanson, B.; Salanne, M.; Rotenberg, B.; Marry, V. Classical Polarizable Force Field to Study Hydrated Hectorite: Optimization on DFT Calculations and Validation against XRD Data. Minerals 2018, 8, 205. https://doi.org/10.3390/min8050205
Hånde R, Ramothe V, Tesson S, Dazas B, Ferrage E, Lanson B, Salanne M, Rotenberg B, Marry V. Classical Polarizable Force Field to Study Hydrated Hectorite: Optimization on DFT Calculations and Validation against XRD Data. Minerals. 2018; 8(5):205. https://doi.org/10.3390/min8050205
Chicago/Turabian StyleHånde, Ragnhild, Vivien Ramothe, Stéphane Tesson, Baptiste Dazas, Eric Ferrage, Bruno Lanson, Mathieu Salanne, Benjamin Rotenberg, and Virginie Marry. 2018. "Classical Polarizable Force Field to Study Hydrated Hectorite: Optimization on DFT Calculations and Validation against XRD Data" Minerals 8, no. 5: 205. https://doi.org/10.3390/min8050205
APA StyleHånde, R., Ramothe, V., Tesson, S., Dazas, B., Ferrage, E., Lanson, B., Salanne, M., Rotenberg, B., & Marry, V. (2018). Classical Polarizable Force Field to Study Hydrated Hectorite: Optimization on DFT Calculations and Validation against XRD Data. Minerals, 8(5), 205. https://doi.org/10.3390/min8050205