Water Interactions with Nanoporous Silica: Comparison of ReaxFF and <i>ab Initio</i> based Molecular Dynamics Simulations

Rimsza, Jessica; Yeon, Jejoon; Duin, Adri C. T. van; Du, Jincheng

doi:10.1021/acs.jpcc.6b07939

Cited by 110 publications

(115 citation statements)

References 90 publications

Supporting

Mentioning

107

Contrasting

Order By: Relevance

“…59 Rimsza et al used DFT-based ab initio MD simulations of waternanoporous silica interactions to validate two versions of ReaxFF potentials for water-silica interactions. 60 It was shown that the new refined model (ReaxFF-2015) can describe the reaction energy barrier of Si-O-Si breakage (hydrolysis reaction) much better than the 2010 version (Fig. 8a).…”

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

confidence: 97%

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

Rimsza

2017

npj Mater Degrad

Self Cite

View full text Add to dashboard Cite

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...

show abstract

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

confidence: 97%

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

Rimsza

2017

npj Mater Degrad

Self Cite

View full text Add to dashboard Cite

show abstract

“…For example, within glass corrosion, classical and ab initio molecular dynamics (MD) simulations are prominently used to generate realistic bulk and surface structures of waste glasses, [215][216][217][218] including the nanoporous gel layer structures during glass corrosion. 219,220 To a lesser degree, MD has also been used to describe ceramics and metal corrosion and inhibition. 221 MD has not been more widely used because of the limited availability of interatomic potentials to describe the heterogeneous interfaces.…”

Section: Silicate Glass Crystalline Ceramic and Metal Corrosion: Simentioning

confidence: 99%

A comparative review of the aqueous corrosion of glasses, crystalline ceramics, and metals

et al. 2018

Self Cite

View full text Add to dashboard Cite

All materials can suffer from environmental degradation; the rate and extent of degradation depend on the details of the material composition and structure as well as the environment. The corrosion of silicate glasses, crystalline ceramics, and metals, particularly as related to nuclear waste forms, has received a lot of attention. The corrosion phenomena and mechanisms of these materials are different, but also have many similarities. This review compares and contrasts the mechanisms of environmental degradation of glass, crystalline ceramics, and metals, with the goal of identifying commonalities that can seed synergistic activities and advance the current knowledge in each area.npj Materials Degradation (2018) 2:15 ; doi:10.1038/s41529-018-0037-2 INTRODUCTIONNew research activity focused on the environmental degradation of silicate glasses, crystalline ceramics, and metals relevant to nuclear waste forms and containers has recently been described.

show abstract

“…use of a reactive potential is critical for analyzing all the reactions and material transport inside the glass and solution. Recent improvements of reactive MD force fields have allowed for several advances in the modeling of silica‐water interactions . In one of the most recent studies of sodium silicate hydration with the ReaxFF, leaching of sodium into water and accumulation at the interface of the leached Na + ions was observed along with proton transport inside the glass in the first nanosecond of reaction.…”

Section: Introductionmentioning

confidence: 99%

“…Recent improvements of reactive MD force fields have allowed for several advances in the modeling of silica-water interactions. [33][34][35][36][37][38] In one of the most recent studies of sodium silicate hydration with the ReaxFF, 39 leaching of sodium into water and accumulation at the interface of the leached Na + ions was observed along with proton transport inside the glass in the first nanosecond of reaction. Another recent study with the same ReaxFF potential studied the continuation of these simulations for a longer time (3 ns) and for different temperatures.…”

mentioning

confidence: 99%

Hydration and reaction mechanisms on sodium silicate glass surfaces from molecular dynamics simulations with reactive force fields

Mahadevan

2020

J Am Ceram Soc

Self Cite

View full text Add to dashboard Cite

Recent development of reactive force fields have enabled molecular dynamics simulations of interactions between silicate glasses and water at the atomistic scale. While multicomponent silicate glasses encompass a wide variety of compositions and properties, one common structural feature in these glasses is the combination of the network structure that is made up of silica tetrahedra linked through corner sharing interspersed with network modifiers like alkali and alkaline‐earth ions that break up the Si–O–Si linkages by forming nonbridging oxygen. In reactions with water, ion exchange between alkali ions in the glass and proton or hydronium in the solution, as well as hydrolysis reaction of the Si–O–Si linkages and subsequent silanol formation, is observed and well documented. We have used a set of recently developed reactive force field to investigate the reactions between water and the surfaces of silica and sodium silicate glasses of different compositions for reactions up to 8 nanoseconds. Our results indicate sodium leaching into water and diffusion of water molecules up to 25 Å into the glass surface. We examined the structural and compositional changes inside the glass and around the diffused ions and use these to explain the rates of silanol formation at the surface. We also observed proton transport in the glass which has an indirect influence on the silanol formation rates. While the surface of the glass was rough to start with, it undergoes further modification into a hydrated gel‐like structure in the glass for up to 5 Å in the higher alkali containing glasses. It was found that the leached sodium ions remain close to the interface and that fragments of silicate network from the surface is capable of dislodging from the bulk glass and enter the aqueous solution. These simulations thus provide insights into the formation and structure of an alteration layers commonly observed in multicomponent silicate glasses corroded in aqueous solutions.

show abstract

Water Interactions with Nanoporous Silica: Comparison of ReaxFF and ab Initio based Molecular Dynamics Simulations

Cited by 110 publications

References 90 publications

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

A comparative review of the aqueous corrosion of glasses, crystalline ceramics, and metals

Hydration and reaction mechanisms on sodium silicate glass surfaces from molecular dynamics simulations with reactive force fields

Contact Info

Product

Resources

About