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Structural and dynamical properties of supercritical H2O-SiO2 fluids studied by ab initio molecular dynamics
- In this study we report the structure of supercritical H2O-SiO2 fluid composed of 50 mol% H2O and 50 mol% SiO2 at 3000 K and 2400 K. investigated by means of ab initio molecular dynamics of models comprising 192 and 96 atoms. The density is set constant to 138 g/cm(3), which yields a pressure of 4.3 GPa at 3000 K and 3.6 GPa at 2400 K. Throughout the trajec[ories, water molecules are formed and dissociated via the network modifying reaction 2 SiOH = SiOSi + H2O The calculation of the reaction constant K- [OH](2)/[H2O][O2-] is carried out on the basis of the experimentally relevant Q ' species notation and agrees well with an extrapolation of experimental data to 3000 K. After quench from 3000 K to 2400 K, the degree of polymerization of the silicate network in the 192-atom models increases noticeably within several tens of picoseconds, accompanied by release of molecular H2O. An unexpected opposite trend is observed in smaller 96-atom models, due to a finite size effect, as several uncorrelated models of 192 and 96 atoms indicate. TheIn this study we report the structure of supercritical H2O-SiO2 fluid composed of 50 mol% H2O and 50 mol% SiO2 at 3000 K and 2400 K. investigated by means of ab initio molecular dynamics of models comprising 192 and 96 atoms. The density is set constant to 138 g/cm(3), which yields a pressure of 4.3 GPa at 3000 K and 3.6 GPa at 2400 K. Throughout the trajec[ories, water molecules are formed and dissociated via the network modifying reaction 2 SiOH = SiOSi + H2O The calculation of the reaction constant K- [OH](2)/[H2O][O2-] is carried out on the basis of the experimentally relevant Q ' species notation and agrees well with an extrapolation of experimental data to 3000 K. After quench from 3000 K to 2400 K, the degree of polymerization of the silicate network in the 192-atom models increases noticeably within several tens of picoseconds, accompanied by release of molecular H2O. An unexpected opposite trend is observed in smaller 96-atom models, due to a finite size effect, as several uncorrelated models of 192 and 96 atoms indicate. The temperature-dependent slowing down of the H2O-silica interaction dynamics is described on the basis of the bond autocorrelation function. (C) 2016 Elsevier B.V. All rights reserved.…
Verfasserangaben: | Georg SpiekermannORCiDGND, Max WilkeORCiDGND, Sandro Jahn |
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DOI: | https://doi.org/10.1016/j.chemgeo.2016.01.010 |
ISSN: | 0009-2541 |
ISSN: | 1878-5999 |
Titel des übergeordneten Werks (Englisch): | Chemical geology : official journal of the European Association for Geochemistry |
Verlag: | Elsevier |
Verlagsort: | Amsterdam |
Publikationstyp: | Wissenschaftlicher Artikel |
Sprache: | Englisch |
Jahr der Erstveröffentlichung: | 2016 |
Erscheinungsjahr: | 2016 |
Datum der Freischaltung: | 22.03.2020 |
Freies Schlagwort / Tag: | DFT; Fluid; Polymerization; SiO(2)Molecular dynamics; SiO2-H2O |
Band: | 426 |
Seitenanzahl: | 10 |
Erste Seite: | 85 |
Letzte Seite: | 94 |
Fördernde Institution: | Mich Supercomputing Centre (JSC) [HPO15]; Deutsche Forschungsgemeinschaft (DFG) from the Emmy-Noether-Program [JA1469/4-1] |
Organisationseinheiten: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Geowissenschaften |
Peer Review: | Referiert |
Name der Einrichtung zum Zeitpunkt der Publikation: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Erd- und Umweltwissenschaften |