Atomic and micro‐structure features of nanoporous aluminosilicate glasses from reactive molecular dynamics simulations

Mahadevan, Thiruvilla S.; Du, Jincheng

doi:10.1111/jace.17465

Cited by 18 publications

(38 citation statements)

References 55 publications

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“…Although its application to glassy systems has thus far remained fairly limited, the ReaxFF forcefield has been used to model several noncrystalline systems, including amorphous silicon [Buehler et al, 2006], glassy silica [Yu et al, 2016], sodium silicate glasses [Deng et al, 2020], modified aluminosilicate glasses [Dongol et al, 2018, Liu et al, 2020c, Mahadevan and Du, 2021, organosilicate glasses [Rimsza et al, 2016], and zeolitic imidazolate frameworks (ZIFs) [Yang et al, 2018], etc. Despite the unique advantages offered by ReaxFF, its applications are presently limited by the range of elements that have been parameterized [Leven et al, 2021, Senftle et al, 2016.…”

Section: Glass Structurementioning

confidence: 99%

Challenges and opportunities in atomistic simulations of glasses: a review

Liu¹,

Zhao²,

Zhou³

et al. 2022

Comptes Rendus. Géoscience

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Atomistic modeling and simulations have been pivotal in our understanding of the glassy state. Indeed, atomistic modeling offers direct access to the structure and dynamics of atoms in glasses-which is typically hidden from conventional experiments. Simulations also offer a more economical, faster alternative to systematic experiments to decode composition-property relationships and accelerate the discovery of new glasses with desirable properties and functionalities. However, the atomistic modeling of glasses remains plagued by a series of challenges, e.g., high computational cost, limited accessible timescale, lack of accurate interatomic forcefields, etc. These challenges often result in the existence of discrepancies between simulation and experimental data, thereby limiting the predictive power of atomistic modeling. Here, we review recent accomplishments and remaining challenges facing the atomistic modeling of glasses. We discuss future opportunities offered by the seamless integration of simulations, knowledge, experiments, and machine learning in advancing glass modeling to a new era.Résumé. La modélisation et simulations atomiques ont joué un rôle important pour notre connaissance de l'état vitreux. En effet, la modélisation atomique offre un accès direct à la structure et dynamique des atomes dans les verres -qui n'est typiquement pas accessible par les techniques expérimentales classiques. Les simulations offrent également une alternative économique et rapide aux expériences systématiques pour décoder les relations composition-propriétés et accélérer la découverte de nouveaux verres offrant des propriétés et fonctionnalités de choix. Cependant, la modélisation atomique des verres reste limitée par une série de défis, par exemple, le coût de calcul élevé, l'échelle de temps accessible limitée, le manque de champs de force interatomiques précis, etc. Ces défis induisent souvent l'existence de divergences entre les résultats simulés et expérimentaux, ce qui limite le pouvoir prédictif de la modélisation atomistique. Dans cette contribution, nous passons en revue les

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Section: Glass Structurementioning

confidence: 99%

Challenges and opportunities in atomistic simulations of glasses: a review

Liu¹,

Zhao²,

Zhou³

et al. 2022

Comptes Rendus. Géoscience

View full text Add to dashboard Cite

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“…180 Further development of the DCRP to include other ions, such as Al and Ca, that are critical to real glass systems (including nuclear waste glasses) would enable MD simulations of the waste glass surface and interfacial reactions with water. 179 This recent development has been applied to study porous calcium aluminosilicate glass (or the dry gel structures) with various porosities and pore morphologies. 179 It will be used to understand hydration, hydrolysis, and water transport in nanoporous calcium aluminosilicate glasses similar to the alteration layer (or gel layer) formed as a result of borosilicate glass corrosion.…”

Section: Formation Structure and Passivation Of The Alteration Layermentioning

confidence: 99%

“…179 This recent development has been applied to study porous calcium aluminosilicate glass (or the dry gel structures) with various porosities and pore morphologies. 179 It will be used to understand hydration, hydrolysis, and water transport in nanoporous calcium aluminosilicate glasses similar to the alteration layer (or gel layer) formed as a result of borosilicate glass corrosion.…”

Section: Formation Structure and Passivation Of The Alteration Layermentioning

confidence: 99%

“…The development of reactive potentials described earlier has enabled the study of the hydrated porous gel structure formed during silicate glass corrosion using MD simulations. Mahadevan and Du modeled the surface hydroxylation of silica as well as the structure and property of bulk water using the two available water–silica potentials: (i) ReaxFF force fields originally developed by van Duin and colleagues − and (ii) diffuse charge-reactive potentials (DCRPs) originally developed for water–silica by Mahadevan and Garofalini and later expanded to include other oxides such as soda, calcia, and alumina by Mahadevan and Du. , It was found that previous ReaxFF parameters for the water–silica system have issues in describing the bulk water properties; however, this was corrected in a newer version of ReaxFF. , The DCRPs were also able to describe the bulk water structure and properties with good accuracy and the water–silica surface reactions as well. One main advantage of the DCRP is their computational efficiency; the approach is ∼10 times faster than ReaxFF.…”

Section: Corrosion Of Glass In Aqueous Environmentsmentioning

confidence: 99%

“…The models subsequently showed that hydration of a sodium silicate glass surface by a layer of water above the glass initiated at certain reactive sites where the water approached the surface following a channel of water until the surface was sufficiently hydroxylated, allowing the remaining water to “pour” down to the surface . Further development of the DCRP to include other ions, such as Al and Ca, that are critical to real glass systems (including nuclear waste glasses) would enable MD simulations of the waste glass surface and interfacial reactions with water . This recent development has been applied to study porous calcium aluminosilicate glass (or the dry gel structures) with various porosities and pore morphologies .…”

Section: Corrosion Of Glass In Aqueous Environmentsmentioning

confidence: 99%

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Recent Advances in Corrosion Science Applicable To Disposal of High-Level Nuclear Waste

et al. 2021

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High-level radioactive waste is accumulating at temporary storage locations around the world and will eventually be placed in deep geological repositories. The waste forms and containers will be constructed from glass, crystalline ceramic, and metallic materials, which will eventually come into contact with water, considering that the period of performance required to allow sufficient decay of dangerous radionuclides is on the order of 105–106 years. Corrosion of the containers and waste forms in the aqueous repository environment is therefore a concern. This Review describes the recent advances of the field of materials corrosion that are relevant to fundamental materials science issues associated with the long-term performance assessment and the design of materials with improved performance, where performance is defined as resistance to aqueous corrosion. Glass, crystalline ceramics, and metals are discussed separately, and the near-field interactions of these different material classes are also briefly addressed. Finally, recommendations for future directions of study are provided.

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