Development of a ReaxFF Reactive Force Field for NaSiO x/Water Systems and Its Application to Sodium and Proton Self-Diffusion

Seung Ho Hahn, Jessica Rimsza, Louise Criscenti, Wei Sun, Lu Deng, Jincheng Du, Tao Liang, Susan B. Sinnott, Adri C.T. Van Duin

Research output: Contribution to journalArticle

8 Citations (Scopus)

Abstract

We present the development of a ReaxFF reactive force field for Na/Si/O/H interactions, which enables reactive molecular dynamics simulation of the sodium silicate-water interfaces. The force field parameters were fitted against various quantum mechanical calculations, including equations of state of different NaSiOx crystalline phases, energy barriers of a sodium cation's transport within the sodium silicate crystal structure, interactions between the hydroxylated silica surface and sodium cation-water systems, and dissociation energies of [NaOH-n(H2O)] (n = 1-6) clusters. After the optimization process, we validated the force field capability through calculating the structures of sodium silicate crystals and glasses and transport properties of sodium ions and protons within the amorphous structures. The force field was also applied to validate the dissociation behavior of sodium hydroxides within the bulk water. Our results with the developed force field are relevant to detailed chemical dissolution mechanisms, which involve (a) the interdiffusion process of sodium ions from glasses and protons from water, (b) subsequent ionic self-diffusion of sodium ions from the subsurface region to vacancy sites at the glass-water interface, and (c) sodium ions interaction with water after leaching from the amorphous sodium silicate system.

Original languageEnglish (US)
Pages (from-to)19613-19624
Number of pages12
JournalJournal of Physical Chemistry C
Volume122
Issue number34
DOIs
StatePublished - Aug 30 2018

Fingerprint

field theory (physics)
Protons
sodium silicates
Sodium
sodium
protons
Water
Ions
water
Silicates
Glass
Cations
glass
ions
dissociation
ionic diffusion
cations
Sodium Hydroxide
sodium hydroxides
Energy barriers

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Cite this

Hahn, Seung Ho ; Rimsza, Jessica ; Criscenti, Louise ; Sun, Wei ; Deng, Lu ; Du, Jincheng ; Liang, Tao ; Sinnott, Susan B. ; Van Duin, Adri C.T. / Development of a ReaxFF Reactive Force Field for NaSiO x/Water Systems and Its Application to Sodium and Proton Self-Diffusion. In: Journal of Physical Chemistry C. 2018 ; Vol. 122, No. 34. pp. 19613-19624.
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Development of a ReaxFF Reactive Force Field for NaSiO x/Water Systems and Its Application to Sodium and Proton Self-Diffusion. / Hahn, Seung Ho; Rimsza, Jessica; Criscenti, Louise; Sun, Wei; Deng, Lu; Du, Jincheng; Liang, Tao; Sinnott, Susan B.; Van Duin, Adri C.T.

In: Journal of Physical Chemistry C, Vol. 122, No. 34, 30.08.2018, p. 19613-19624.

Research output: Contribution to journalArticle

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T1 - Development of a ReaxFF Reactive Force Field for NaSiO x/Water Systems and Its Application to Sodium and Proton Self-Diffusion

AU - Hahn, Seung Ho

AU - Rimsza, Jessica

AU - Criscenti, Louise

AU - Sun, Wei

AU - Deng, Lu

AU - Du, Jincheng

AU - Liang, Tao

AU - Sinnott, Susan B.

AU - Van Duin, Adri C.T.

PY - 2018/8/30

Y1 - 2018/8/30

N2 - We present the development of a ReaxFF reactive force field for Na/Si/O/H interactions, which enables reactive molecular dynamics simulation of the sodium silicate-water interfaces. The force field parameters were fitted against various quantum mechanical calculations, including equations of state of different NaSiOx crystalline phases, energy barriers of a sodium cation's transport within the sodium silicate crystal structure, interactions between the hydroxylated silica surface and sodium cation-water systems, and dissociation energies of [NaOH-n(H2O)] (n = 1-6) clusters. After the optimization process, we validated the force field capability through calculating the structures of sodium silicate crystals and glasses and transport properties of sodium ions and protons within the amorphous structures. The force field was also applied to validate the dissociation behavior of sodium hydroxides within the bulk water. Our results with the developed force field are relevant to detailed chemical dissolution mechanisms, which involve (a) the interdiffusion process of sodium ions from glasses and protons from water, (b) subsequent ionic self-diffusion of sodium ions from the subsurface region to vacancy sites at the glass-water interface, and (c) sodium ions interaction with water after leaching from the amorphous sodium silicate system.

AB - We present the development of a ReaxFF reactive force field for Na/Si/O/H interactions, which enables reactive molecular dynamics simulation of the sodium silicate-water interfaces. The force field parameters were fitted against various quantum mechanical calculations, including equations of state of different NaSiOx crystalline phases, energy barriers of a sodium cation's transport within the sodium silicate crystal structure, interactions between the hydroxylated silica surface and sodium cation-water systems, and dissociation energies of [NaOH-n(H2O)] (n = 1-6) clusters. After the optimization process, we validated the force field capability through calculating the structures of sodium silicate crystals and glasses and transport properties of sodium ions and protons within the amorphous structures. The force field was also applied to validate the dissociation behavior of sodium hydroxides within the bulk water. Our results with the developed force field are relevant to detailed chemical dissolution mechanisms, which involve (a) the interdiffusion process of sodium ions from glasses and protons from water, (b) subsequent ionic self-diffusion of sodium ions from the subsurface region to vacancy sites at the glass-water interface, and (c) sodium ions interaction with water after leaching from the amorphous sodium silicate system.

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