Dissociative Water Potential for Molecular Dynamics Simulations

Mahadevan, Thiruvilla S.; Garofalini, Stephen H.

doi:10.1021/jp072530o

Cited by 135 publications

(205 citation statements)

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“…52 Recently, Mahadevan and Garofalini developed a dissociative water-silica forcefield based on water potentials by Guillot and Guissani. 53 Another forcefield used the BKS potential for silica and a SPC/E water model with Buckingham interactions for water-silica interfaces was developed by Hassanali and Singer. 54 Other water-silica potentials have been developed; 55,56 however, truly reactive potentials that can describe silica and water structures, reaction pathways, and energetics are rare.…”

Section: First-principles-based Simulations Of Glass-water Interactionsmentioning

confidence: 99%

“…Dissociation energy barriers of different Si Q n species (silicon oxygen tetrahedron with n bridging oxygen) on silica glass surfaces were investigated using the potential mean force approach with MD simulations. By using the dissociative watersilica potential developed by Mahadevan and Garofalini, 53 it was found that among the four (Q 4 → Q 3 , Q 3 → Q 2 , Q 2 → Q 1 , or Q 1 → Q 0 ) reactions, the Q 3 → Q 2 and Q 2 → Q 1 reactions have the highest activation energy of~14.1 kcal/mol, and is the rate limiting step in bulk silica dissolution. 19,24 These barriers are in the lower range of the experimental energy barriers of 14-24 kcal/mol and below values from cluster-based ab initio calculations (18-39 kcal/ mol).…”

Section: First-principles-based Simulations Of Glass-water Interactionsmentioning

confidence: 99%

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Atomistic computer simulations of water interactions and dissolution of inorganic glasses

Rimsza

2017

npj Mater Degrad

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Computer simulations at the atomistic scale play an increasing important role in understanding the structure features, and the structure-property relationships of glass and amorphous materials. In this paper, we reviewed atomistic simulation methods ranging from first principles calculations and ab initio molecular dynamics (AIMD) simulations, to classical molecular dynamics (MD), and meso-scale kinetic Monte Carlo (KMC) simulations and their applications to study the reactions and interactions of inorganic glasses with water and the dissolution behaviors of inorganic glasses. Particularly, the use of these simulation methods in understanding the reaction mechanisms of water with oxide glasses, water-glass interfaces, hydrated porous silica gels formation, the structure and properties of multicomponent glasses, and microstructure evolution are reviewed. The advantages and disadvantageous of these simulation methods are discussed and the current challenges and future direction of atomistic simulations in glass dissolution presented.npj Materials Degradation (2017) 1:16 ; doi:10.1038/s41529-017-0017-yThe corrosion or degradation of glasses in aqueous solutions are critical in a number of engineering and technological processes ranging from microelectronic packaging, glass reaction chambers, and the immobilization of nuclear waste materials, as well as in healthcare and biomedical fields such as dissolution of inhaled glass fibers and bioactive glasses for biomedical applications. In particular, immobilizing radioactive waste in borosilicate glasses is widely accepted as a preferred method to treat nuclear waste materials generated from civilian and military sources. This process, also known as vitrification, is a critical component of the cycle of nuclear energy to combat global environmental and energy challenges. Researchers from around the world have extensively invested in understanding glass corrosion in an effort to predict the long-term stability and release rate radionuclides to the environment during nuclear waste storage. 1,2Various mechanisms for glass corrosion have been proposed and despite intensive experimental investigations with advanced characterization techniques results are unclear. It is generally accepted that the corrosion of glass consists of a set of complex processes including hydration, hydrolysis, and ion-exchange that are coupled during glass dissolution. The initial stage is interdiffusion of proton or hydronium ions from the solution with sodium or other alkali ions in the glass.3 This is followed by the hydrophilic attack of water on the Si-O-Si or Si-O-Al linkages that lead to hydroxylation of the silicate glass network. The remaining hydrolyzed glass skeleton then undergoes condensation and repolymerization to form the hydrated nanoporous silica rich gel layer which can be protective, decreasing dissolution to a residual rate. [4][5][6] The morphology of the gel layer, such as thickness, pore structure, and chemical composition, depends on the original glass composition and the pH...

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Section: First-principles-based Simulations Of Glass-water Interactionsmentioning

confidence: 99%

Section: First-principles-based Simulations Of Glass-water Interactionsmentioning

confidence: 99%

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

Rimsza

2017

npj Mater Degrad

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“…A second assumption is that currently available classical (e.g, Pedone et al, 2008) and reactive force field models (Garofalini, 2001;Mahadevan and Garofalini, 2007;2008) can effectively be used to model the multicomponent glass structures and surfaces proposed for study. There is a possibility that additional force field development will be required.…”

Section: Overall Approachmentioning

confidence: 99%

Progress toward bridging from atomistic to continuum modeling to predict nuclear waste glass dissolution.

Zapol

Bourg

Criscenti³

et al. 2011

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This report summarizes research performed for the Nuclear Energy Advanced Modeling and Simulation (NEAMS) Subcontinuum and Upscaling Task. The work conducted focused on developing a roadmap to include molecular scale, mechanistic information in continuum-scale models of nuclear waste glass dissolution. This information is derived from molecular-scale modeling efforts that are validated through comparison with experimental data. In addition to developing a master plan to incorporate a subcontinuum mechanistic understanding of glass dissolution into continuum models, methods were developed to generate constitutive dissolution rate expressions from quantum calculations, force field models were selected to generate multicomponent glass structures and gel layers, classical molecular modeling was used to study diffusion through nanopores analogous to those in the interfacial gel layer, and a micro-continuum model (KµC) was developed to study coupled diffusion and reaction at the glass-gel-solution interface. We would also like to acknowledge discussions with the International Corrosion Working Group members including Stéphane Gin,

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“…Up to this point, the presentation covered only nontitratable water models. The parametrization of good dissociative water potentials (and their combination with force fields parameters for the other molecular species) is another critical issue and open question (Mahadevan and Garofalini 2008). In the same line, it has not been proven yet that the classical force fields parameters obtained at a given fixed experimental pH and salt conditions and routinely used to study the biomolecular phenomena are valid to explore all other interesting physical chemical regimes different than the ones used in the calibration process.…”

Section: Introductionmentioning

confidence: 99%

Development of constant-pH simulation methods in implicit solvent and applications in biomolecular systems

daSilva

Dias

2017

Biophys Rev

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pH is a critical parameter for biological and technological systems directly related with electrical charges. It can give rise to peculiar electrostatic phenomena, which also makes them more challenging. Due to the quantum nature of the process, involving the forming and breaking of chemical bonds, quantum methods should ideally by employed. Nevertheless, due to the very large number of ionizable sites, different macromolecular conformations, salt conditions, and all other charged species, the CPU time cost simply becomes prohibitive for computer simulations, making this a quite complex problem. Simplified methods based on Monte Carlo sampling have been devised and will be reviewed here, highlighting the updated state-ofthe-art of this field, advantages, and limitations of different theoretical protocols for biomolecular systems (proteins and nucleic acids). Following a historical perspective, the discussion will be associated with the applications to protein interactions with other proteins, polyelectrolytes, and nanoparticles.

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Dissociative Water Potential for Molecular Dynamics Simulations

Cited by 135 publications

References 38 publications

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

Progress toward bridging from atomistic to continuum modeling to predict nuclear waste glass dissolution.

Development of constant-pH simulation methods in implicit solvent and applications in biomolecular systems

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