NaCl nucleation from brine in seeded simulations: Sources of uncertainty in rate estimates

Zimmermann, Nils. E. R. and Vorselaars, Bart and Espinosa, Jorge R. and Quigley, David and Smith, William R. and Sanz, Eduardo and Vega, Carlos and Peters, Baron (2018) NaCl nucleation from brine in seeded simulations: Sources of uncertainty in rate estimates. The Journal of Chemical Physics, 148 (22). p. 222838. ISSN 0021-9606

Full content URL: http://doi.org/10.1063/1.5024009

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Item Type:Article
Item Status:Live Archive

Abstract

This work reexamines seeded simulation results for NaCl nucleation from a supersaturated aqueous solution at 298.15 K and 1 bar pressure. We present a linear regression approach for analyzing seeded simulation data that provides both nucleation rates and uncertainty estimates. Our results show that rates obtained from seeded simulations rely critically on a precise driving force for the model system. The driving force vs. solute concentration curve need not exactly reproduce that of the real system, but it should accurately describe the thermodynamic properties of the model system. We also show that rate estimates depend strongly on the nucleus size metric. We show that the rate estimates systematically increase as more stringent local order parameters are used to count members of a cluster and provide tentative suggestions for appropriate clustering criteria.

Keywords:Crystallography, Brines, Electrolytes, Molecular dynamics, linear regression, adsorption, Computer simulation, thermodynamic properties
Subjects:F Physical Sciences > F310 Applied Physics
F Physical Sciences > F300 Physics
F Physical Sciences > F200 Materials Science
F Physical Sciences > F170 Physical Chemistry
F Physical Sciences > F343 Computational Physics
Divisions:College of Science > School of Mathematics and Physics
ID Code:32236
Deposited On:27 Jun 2018 20:44

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