Molecular Dynamics Investigation of Halide-Containing Phospho-Silicate Bioactive Glasses

Pedone, Alfonso; Chen, Xiaojing; Hill, Robert G.; Karpukhina, Natalia

doi:10.1021/acs.jpcb.8b00547

Cited by 29 publications

(21 citation statements)

References 40 publications

(85 reference statements)

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“…QSPR analysis is a powerful approach developed in biological sciences to find optimal correlations between macroscopic properties and descriptors based on microstructure features 19 . QSPR has been applied to materials to find structure‐property relationship in polymers 20–28 and glass materials 19,29–34 . It has been shown particularly powerful when QSPR analysis is combined with MD simulations, where various structural and energetic information can be extracted for complex systems, to correlate experimental measured properties (e.g., r 0 of Zr‐containing borosilicate glasses 33 and physical properties of calcium aluminosilicate glasses 34 ).…”

Section: Introductionmentioning

confidence: 99%

Predicting the dissolution rate of borosilicate glasses using QSPR analysis based on molecular dynamics simulations

Gin

et al. 2021

J Am Ceram Soc

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Quantitative Structure Property Relationship (QSPR) analysis based on molecular dynamics (MD) simulations is a promising approach for establishing the composition‐property relationships of glasses and other materials with complex structures. A series of 20 borosilicate, aluminosilicate, and boroaluminosilicate glasses have been modeled using MD simulations with recently developed effective potentials. Short‐ and medium‐range structures of these glasses were analyzed and, based on the structural information, QSPR analysis of the initial dissolution rates (r0) of these glasses that were measured at 90°C and pH 9 by using various structural descriptors such as percentage of bridging oxygen species, network connectivity, and average ring size. The structural descriptor, Fnet, which contains both energetic information such as single bond strength and structural information such as cation coordination number and Qn distribution, was also used. It was found that while the overall network connectivity, average ring size and Fnet provide reasonable correlations with r0 of studied glasses, Fnet gives the best correlation among the descriptors. For glasses that show incongruent dissolution, it was found that modification of glass compositions to account for preferential release of modifier cations is necessary to achieve best correlations. The findings were discussed with results of recent studies on evaluating the compositional dependence of glass dissolution behavior using the topological‐constraints‐based models.

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Section: Introductionmentioning

confidence: 99%

Predicting the dissolution rate of borosilicate glasses using QSPR analysis based on molecular dynamics simulations

Gin

et al. 2021

J Am Ceram Soc

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“…MD simulation has been proved to be an efficient method to understand the glass structure and structure–property relations from atomic level . Recently, with the development of empirical potentials, glass systems with multiple anions (such as O/F, , O/Cl , ) have been studied and the results are found to be in favorable comparison with the experiments. In our earlier study, phase separation into the oxide-rich phase consisting [SiO 4 ] and [AlO 4 ] formers and in the fluoride-rich phase with modifier enriching was observed with the help of MD simulations. , The compositions in fluoride-rich regions are in good agreement with those in the precipitated crystal phases observed in experiments.…”

Section: Introductionmentioning

confidence: 99%

Structural Origins of RF₃/NaRF₄ Nanocrystal Precipitation from Phase-Separated SiO₂–Al₂O₃–RF₃–NaF Glasses: A Molecular Dynamics Simulation Study

Zhao

et al. 2019

J. Phys. Chem. B

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Oxyfluoride glass-ceramics with RF3 or NaRF4 (R3+: rare earth elements) nanocrystals are considered as favorable hosts for luminescence applications. In this work, we utilized large-scale molecular dynamics (MD) simulations with effective partial charge potentials to study a series of oxyfluoride glasses that are of interest to the precipitation of RF3 or NaRF4 nanocrystals as previous experiment results suggested. The results show that phase separation exists in all glass compositions with fluoride-rich regions made up of R3+, Na+, and F– and oxide-rich regions consisting of aluminosilicate networks. These fluoride-enriched regions can serve as the precursor for RF3, cubic and hexagonal NaRF4, and NaF crystal precipitation. The results also confirm that the concentration of Na+ in the fluoride phase plays a key role in determining the crystal phases (RF3, NaRF4, or NaF) and crystal structure (cubic vs hexagonal NaRF4) to be precipitated. Consequently, this study shows that MD simulations with effective potentials can fill the gap in the structural understanding of oxyfluoride glass and provide insights into atomic scale information of the phase separation behavior that is useful in predicting the potential crystal types in oxyfluoride glass. When coupled with experimental validations, these simulations can expedite the exploration of novel luminescent oxyfluoride glass ceramics.

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“…It is well known that the accuracy of the MD simulation results in describing the structure and properties of materials (inorganic glasses in this context) strongly depends on the interatomic potential models used to obtain forces between ions for the integration of the equation of motion. In the last decades, a variety of interatomic potentials for the different families of oxide glasses (silicates, aluminosilicates, borosilicate, phosphosilicate etc…) have been developed [20][21][22][23][24][25][26][27][28][29][30] . The majority of them were optimized by fitting on experimental data, whereas the others adopted quantum mechanical data (usually coming from ab initio MD simulations) 26,30 .…”

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confidence: 99%

Structural origins of the Mixed Alkali Effect in Alkali Aluminosilicate Glasses: Molecular Dynamics Study and its Assessment

Lodesani

Menziani

Hijiya³

et al. 2020

Sci Rep

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The comprehension of the nonlinear effects provided by mixed alkali effect (MAE) in oxide glasses is useful to optimize glass compositions to achieve specific properties that depend on the mobility of ions, such as the chemical durability, glass transition temperature, viscosity and ionic conductivity. Although molecular dynamics (MD) simulations have already been applied to investigate the MAE on silicates, less effort has been devoted to study such phenomenon in mixed alkali aluminosilicate glasses where alkali cations can act both as modifiers, forming non-bridging oxygens and percolation channels, and as charge compensator of the Alo 4 − units present in the network. Moreover, the ionic conductivity has not been computed yet; thus, the accuracy of the atomistic simulations in reproducing the MAE on the property is still open to question. In this work, we have validated five major interatomic potentials for the classical MD simulations by modelling the structure, density, glass transition temperature and ionic conductivity for three aluminosilicate glasses, (25 − x)Na 2 o − x(K 2 O) − 10(Al 2 o 3) − 65(SiO 2) (x = 0, 12.5, 25). It was observed that only the core-shell (CS) polarizable force field well reproduces the experimentally measured MAe on T g and the ionic conductivity as well as the higher conductivity of single sodium aluminosilicate glass at low temperature and the higher conductivity of single potassium aluminosilicate glass at high temperature. The MAE is related to the suppression of jump events of the alkaline ions between dissimilar sites in the percolation channels consisting of both sodium and potassium ions as in the case of alkaline silicates. The superior reproducibility of the CS potential is originated from the larger and the flexible ring structures due to the smaller Si-O-Si inter-tetrahedra angle, creating appropriate percolation channels for ion conductivity. We also report detailed assessments for using the potential models including the CS potential for investigating MAE on aluminosilicates. Ionic conductivity in inorganic glasses is gaining a huge interest for the enormous number of applications that such materials are having in a number of major technological developments in the domains of energy conversion and storage (solid electrolytes in battery and fuel cells) or in the environmental monitoring (solid state ionic membranes for sensors) 1. Among the various ways to control ionic diffusion and thus ionic conductivity a possibility is that to exploit the so-called Mixed Alkali Effect (MAE) or more in general the Mixed Ion Effect (MIE) 2,3. This effect refers to a large non-linear deviation in glass properties observed when an alkali cation (or more in general a mobile ion) is gradually replaced by another alkali cation. The ionic conductivity of glasses exhibiting the MAE shows a deep minimum when half of the alkaline ions of type A are replaced by type B ions, meaning that cation mobility progressively reduces up to a substitution ratio equal to unity. The minimum is more pron...

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Molecular Dynamics Investigation of Halide-Containing Phospho-Silicate Bioactive Glasses

Cited by 29 publications

References 40 publications

Predicting the dissolution rate of borosilicate glasses using QSPR analysis based on molecular dynamics simulations

Predicting the dissolution rate of borosilicate glasses using QSPR analysis based on molecular dynamics simulations

Structural Origins of RF₃/NaRF₄ Nanocrystal Precipitation from Phase-Separated SiO₂–Al₂O₃–RF₃–NaF Glasses: A Molecular Dynamics Simulation Study

Structural origins of the Mixed Alkali Effect in Alkali Aluminosilicate Glasses: Molecular Dynamics Study and its Assessment

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Molecular Dynamics Investigation of Halide-Containing Phospho-Silicate Bioactive Glasses

Cited by 29 publications

References 40 publications

Predicting the dissolution rate of borosilicate glasses using QSPR analysis based on molecular dynamics simulations

Predicting the dissolution rate of borosilicate glasses using QSPR analysis based on molecular dynamics simulations

Structural Origins of RF3/NaRF4 Nanocrystal Precipitation from Phase-Separated SiO2–Al2O3–RF3–NaF Glasses: A Molecular Dynamics Simulation Study

Structural origins of the Mixed Alkali Effect in Alkali Aluminosilicate Glasses: Molecular Dynamics Study and its Assessment

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Structural Origins of RF₃/NaRF₄ Nanocrystal Precipitation from Phase-Separated SiO₂–Al₂O₃–RF₃–NaF Glasses: A Molecular Dynamics Simulation Study