Computational Modeling of Silicate Glasses: A Quantitative Structure-Property Relationship Perspective

Pedone, Alfonso; Menziani, Maria Cristina

doi:10.1007/978-3-319-15675-0_5

Cited by 21 publications

(56 citation statements)

References 87 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…In general, a good agreement is observed denoting that the DFT refinement of the MD-generated structural models reproduces the boron environment fairly well. In particular, the areas underlying the BO 3 ≡ B [3] and BO 4 ≡ B [4] peaks observed respectively at 10-20 ppm and around 0 ppm are in nice agreement for B18.4 and B37.5 glasses generated with Bauchy and Du potentials denoting a good repartition between the B [3] and B [4] species in the models. The agreement with experiments is worse for the B56.25 and B75 glasses.…”

Section: Resultssupporting

confidence: 58%

“…The agreement with experiments is worse for the B56.25 and B75 glasses. It is worth noting that the shape and the broadening of the B [4] peak are very well reproduced for all the glasses and all potentials whereas some discrepancies are observed for that of the B [3] species. In particular, the B [3] peak of the simulated spectra of the models generated with the Bauchy and Du potentials is shifted to less positive chemical shifts when compared with the corresponding experimental results.…”

Section: Resultsmentioning

confidence: 78%

“…Therefore, a new level of conceptual understanding about the compositional and structural dependence of dissolution behavior and other properties of boron‐containing glasses is required that can be applied to attain a significant leap in the design of glasses suitable for specific applications. In the field of bioactive glasses, one major challenge that decelerates the design and development of boron‐containing bioactive glasses with controlled corrosion behavior is the lack of reliable computational models to decipher the structural descriptors for these glasses which, upon convergence with the experimental data on glass dissolution, can be used to develop predictive Quantitative Structure‐Property Relationship models …”

Section: Introductionmentioning

confidence: 99%

“…In the field of bioactive glasses, one major challenge that decelerates the design and development of boron-containing bioactive glasses with controlled corrosion behavior is the lack of reliable computational models to decipher the structural descriptors for these glasses which, upon convergence with the experimental data on glass dissolution, can be used to develop predictive Quantitative Structure-Property Relationship models. 3,4 In the last decades, considerable achievements have been made in using classical molecular dynamics simulations to predict glass structure and properties. [5][6][7][8] However, exploring the structure of boron-containing glasses through atomistic simulations has been historically a challenge due to the complexity of boron-oxygen bonding (which is not only partially covalent but also allows the boron coordination in glass to change with composition as shown in Equations [1] and [2]) and its dependence on the thermal history of glass.…”

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Assessment of interatomic parameters for the reproduction of borosilicate glass structures via DFT‐GIPAW calculations

et al. 2019

Self Cite

View full text Add to dashboard Cite

Borates and borosilicates are potential candidates for the design and development of glass formulations with important industrial and technological applications. A major challenge that retards the pace of development of borate/borosilicate based glasses using predictive modeling is the lack of reliable computational models to predict the structure‐property relationships in these glasses over a wide compositional space. A major hindrance in this pursuit has been the complexity of boron‐oxygen bonding due to which it has been difficult to develop adequate B–O interatomic potentials. In this article, we have evaluated the performance of three B–O interatomic potential models recently developed by Bauchy et al [J. Non‐Cryst. Solids, 2018, 498, 294–304], Du et al [J. Am. Ceram. Soc. https://doi.org/10.1111/jace.16082] and Edèn et al [Phys. Chem. Chem. Phys., 2018, 20, 8192–8209] aiming to reproduce the short‐to‐medium range structures of sodium borosilicate glasses in the system 25 Na2O x B2O3 (75 − x) SiO2 (x = 0‐75 mol%). To evaluate the different force fields, we have computed at the density functional theory level the NMR parameters of 11B, 23Na, and 29Si of the models generated with the three potentials and the simulated MAS NMR spectra compared with the experimental counterparts. It was observed that the rigid ionic models proposed by Bauchy and Du can both reliably reproduce the partitioning between BO3 and BO4 species of the investigated glasses, along with the local environment around sodium in the glass structure. However, they do not accurately reproduce the second coordination sphere of silicon ions and the Si–O–T (T = Si, B) and B‐O‐T distribution angles in the investigated compositional space which strongly affect the NMR parameters and final spectral shape. On the other hand, the core‐shell parameterization model proposed by Edén underestimates the fraction of BO4 species of the glass with composition 25Na2O 18.4B2O3 56.6SiO2 but can accurately reproduce the shape of the 11B and 29Si MAS‐NMR spectra of the glasses investigations due to the narrower B–O–T and Si‐O‐T bond angle distributions. Finally, the effect of the number of boron atoms (also distinguishing the BO3 and BO4 units) in the second coordination sphere of the network former cations on the NMR parameters have been evaluated.

show abstract

Section: Resultssupporting

confidence: 58%

Section: Resultsmentioning

confidence: 78%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Assessment of interatomic parameters for the reproduction of borosilicate glass structures via DFT‐GIPAW calculations

et al. 2019

Self Cite

View full text Add to dashboard Cite

show abstract

“…The structure of these glasses can be described by a modified random network where the network of mostly corner sharing silica tetrahedra is interspersed with channels of modifier alkali or alkaline earth cations forming nonbridging oxygens (NBO's). Recent developments lead to high technology applications of silicate glasses in fields such as display, photonics, biomedicine, and for the immobilization and containment of nuclear waste materials by vitrification. Although the glass compositions used for these applications are more complicated such as phosposilicate, aluminosilicate and borosilicates, sodium silicate glasses can serve as a representative model for such multicomponent silicate glasses and are the subject of a range of experimental and simulation studies .…”

Section: Introductionmentioning

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

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

Rare Earth and Transition Metal Containing Glasses

Du¹,

Montorsi²,

Barbi³

et al. 2022

Atomistic Simulations of Glasses

View full text Add to dashboard Cite

Computational Modeling of Silicate Glasses: A Quantitative Structure-Property Relationship Perspective

Cited by 21 publications

References 87 publications

Assessment of interatomic parameters for the reproduction of borosilicate glass structures via DFT‐GIPAW calculations

Assessment of interatomic parameters for the reproduction of borosilicate glass structures via DFT‐GIPAW calculations

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

Rare Earth and Transition Metal Containing Glasses

Contact Info

Product

Resources

About