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

Mahadevan, Thiruvilla S.; Du, Jincheng

doi:10.1111/jace.17465

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

Journal Article · Mon Sep 07 00:00:00 EDT 2020 · Journal of the American Ceramic Society

DOI:https://doi.org/10.1111/jace.17465· OSTI ID:1902999

Mahadevan, Thiruvilla S. ^[1]; ^[2]

Univ. of North Texas, Denton, TX (United States); University of North Texas
Univ. of North Texas, Denton, TX (United States)

Long-term chemical durability of borosilicate glasses that makes them a widely accepted form of nuclear waste disposal is achieved through the formation of a porous aluminosilicate gel layer that provides passivity and limits the transport of water to the reaction front. Detailed understanding of the porous silicate gel layer is thus critical in elucidating the corrosion mechanism of these glasses and to design of new glass composition for waste immobilization and other applications. In this paper, we use the diffuse charge reactive potential to generate porous aluminosilicate glass structures with compositions equivalent to the gel layers formed at the glass-water interface with an aim to understand the processing condition on the microstructure and atomic structure of these systems. We demonstrate the use of the charge scaling techniques is an effective approach to generate these porous structures with controllable pore mophologies. After initial validation of the potentials and calcium aluminosilicate glass structures using neutron diffraction, we created gel structures with compositions similar to well-known model nuclear waste borosilicate glasses. The porosities and the pore size distribution bear a strong correlation to the processing temperature, as well as to the local atomic structure. Thus, by controlling the processing parameters, the generated porous structures can be customized to closely resemble gel structures due to borosilicate glass corrosion. Furthermore, these results provide insights of the micro- and atomic structure features of the porous aluminosilicate glasses and on the optimal procedure to generate porous structures that can be comparable to experimentally observed gel layer structures thus to elaborate on the correlations between the structure and phenomena in glass-water interactions.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of North Texas, Denton, TX (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0016584

OSTI ID:: 1902999

Alternate ID(s):: OSTI ID: 1852332
OSTI ID: 1787122

Journal Information:: Journal of the American Ceramic Society, Journal Name: Journal of the American Ceramic Society Journal Issue: 1 Vol. 104; ISSN 0002-7820

Publisher:: American Ceramic SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (53)

Molecular Mechanisms Causing Anomalously High Thermal Expansion of Nanoconfined Water Garofalini, Stephen H.; Mahadevan, Thiruvilla S.; Xu, Shuangyan ChemPhysChem, Vol. 9, Issue 14 https://doi.org/10.1002/cphc.200800455	journal	October 2008
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Neutron and X-ray amorphography Wright, Adrian C. Journal of Non-Crystalline Solids, Vol. 106, Issue 1-3 https://doi.org/10.1016/0022-3093(88)90218-9	journal	December 1988
Neutron scattering from vitreous silica IV. Time-of-flight diffraction Grimley, David I.; Wright, Adrian C.; Sinclair, Roger N. Journal of Non-Crystalline Solids, Vol. 119, Issue 1 https://doi.org/10.1016/0022-3093(90)90240-M	journal	March 1990
The comparison of molecular dynamics simulations with diffraction experiments Wright, Adrian C. Journal of Non-Crystalline Solids, Vol. 159, Issue 3 https://doi.org/10.1016/0022-3093(93)90232-M	journal	January 1993
Points of contact between theory and experiment: a comparison of molecular dynamics and neutron diffraction results Cao, Yuan; Cormack, Alastair N.; Clare, Alexis G. Journal of Non-Crystalline Solids, Vol. 177 https://doi.org/10.1016/0022-3093(94)90545-2	journal	November 1994
Alkali silicate glasses: interpreting neutron diffraction results using the molecular dynamics simulation technique Vessal, Behnam; Wright, Adrian C.; Hannon, Alex C. Journal of Non-Crystalline Solids, Vol. 196 https://doi.org/10.1016/0022-3093(95)00592-7	journal	March 1996
VMD: Visual molecular dynamics Humphrey, William; Dalke, Andrew; Schulten, Klaus Journal of Molecular Graphics, Vol. 14, Issue 1 https://doi.org/10.1016/0263-7855(96)00018-5	journal	February 1996
Molecular dynamics simulation of nanoporous silica Beckers, J. V. L.; de Leeuw, S. W. Journal of Non-Crystalline Solids, Vol. 261, Issue 1-3 https://doi.org/10.1016/S0022-3093(99)00607-9	journal	January 2000
Modifications of the hydrogen bond network of liquid water in a cylindrical SiO2 pore Hartnig, Christoph; Witschel, Wolfgang; Spohr, Eckhard Journal of Molecular Liquids, Vol. 85, Issue 1-2 https://doi.org/10.1016/S0167-7322(99)00169-5	journal	April 2000
Efficient algorithm for primitive ring statistics in topological networks Yuan, Xianglong; Cormack, A. N. Computational Materials Science, Vol. 24, Issue 3 https://doi.org/10.1016/S0927-0256(01)00256-7	journal	June 2002
Porous structure of natural and modified clinoptilolites Kowalczyk, Piotr; Sprynskyy, Myroslav; Terzyk, Artur P. Journal of Colloid and Interface Science, Vol. 297, Issue 1 https://doi.org/10.1016/j.jcis.2005.10.045	journal	May 2006
An overview on silica aerogels synthesis and different mechanical reinforcing strategies Maleki, Hajar; Durães, Luisa; Portugal, António Journal of Non-Crystalline Solids, Vol. 385 https://doi.org/10.1016/j.jnoncrysol.2013.10.017	journal	February 2014
Thermal properties, density and structure of percalcic and peraluminus CaO–Al2O3–SiO2 glasses Takahashi, Shoji; Neuville, Daniel R.; Takebe, Hiromichi Journal of Non-Crystalline Solids, Vol. 411 https://doi.org/10.1016/j.jnoncrysol.2014.12.019	journal	March 2015
Neutron diffraction of calcium aluminosilicate glasses and melts Hennet, Louis; Drewitt, James W. E.; Neuville, Daniel R. Journal of Non-Crystalline Solids, Vol. 451 https://doi.org/10.1016/j.jnoncrysol.2016.05.018	journal	November 2016
An international initiative on long-term behavior of high-level nuclear waste glass Gin, S.; Abdelouas, A.; Criscenti, L. J. Materials Today, Vol. 16, Issue 6 https://doi.org/10.1016/j.mattod.2013.06.008	journal	June 2013
Application of natural zeolites in environmental remediation: A short review Misaelides, Panagiotis Microporous and Mesoporous Materials, Vol. 144, Issue 1-3 https://doi.org/10.1016/j.micromeso.2011.03.024	journal	October 2011
Open Scientific Questions about Nuclear Glass Corrosion Gin, S. Procedia Materials Science, Vol. 7 https://doi.org/10.1016/j.mspro.2014.10.022	journal	January 2014
Development of Water Reactive Potentials for Sodium Silicate Glasses Mahadevan, Thiruvilla S.; Sun, Wei; Du, Jincheng The Journal of Physical Chemistry B, Vol. 123, Issue 20 https://doi.org/10.1021/acs.jpcb.9b02216	journal	April 2019
Interfacial Structure and Evolution of the Water–Silica Gel System by Reactive Force-Field-Based Molecular Dynamics Simulations Rimsza, J. M.; Du, Jincheng The Journal of Physical Chemistry C, Vol. 121, Issue 21 https://doi.org/10.1021/acs.jpcc.7b02734	journal	May 2017
Molecular Dynamics Simulations of Water Structure and Diffusion in a 1 nm Diameter Silica Nanopore as a Function of Surface Charge and Alkali Metal Counterion Identity Collin, Marie; Gin, Stéphane; Dazas, Baptiste The Journal of Physical Chemistry C, Vol. 122, Issue 31 https://doi.org/10.1021/acs.jpcc.8b03902	journal	July 2018
Reaction Mechanisms and Interfacial Behaviors of Sodium Silicate Glass in an Aqueous Environment from Reactive Force Field-Based Molecular Dynamics Simulations Deng, Lu; Miyatani, Katsuaki; Amma, Shin-ichi The Journal of Physical Chemistry C, Vol. 123, Issue 35 https://doi.org/10.1021/acs.jpcc.9b05030	journal	August 2019
Particle Release and Permeability Reduction in a Natural Zeolite (Clinoptilolite) and Sand Porous Medium Abadzic, S. Dean; Ryan, Joseph N. Environmental Science & Technology, Vol. 35, Issue 22 https://doi.org/10.1021/es001868s	journal	November 2001
Oligomerization in silica sols Feuston, B. P.; Garofalini, S. H. The Journal of Physical Chemistry, Vol. 94, Issue 13 https://doi.org/10.1021/j100376a035	journal	June 1990
Surface-to-Volume Ratio of Porous Materials Obtained by a Combined Use of NMR and MIP Hansen, E. W.; Gran, H. C.; Kvernberg, P. O. The Journal of Physical Chemistry B, Vol. 101, Issue 45 https://doi.org/10.1021/jp971925c	journal	November 1997
Fast Method for Computing Pore Size Distributions of Model Materials Bhattacharya, Supriyo; Gubbins, Keith E. Langmuir, Vol. 22, Issue 18 https://doi.org/10.1021/la052651k	journal	August 2006
Pore Size Distributions in Porous Glasses: A Computer Simulation Study Gelb, Lev D.; Gubbins, K. E. Langmuir, Vol. 15, Issue 2 https://doi.org/10.1021/la9808418	journal	January 1999
Dynamics of self-reorganization explains passivation of silicate glasses Gin, Stéphane; Collin, Marie; Jollivet, Patrick Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04511-2	journal	June 2018
Structure of International Simple Glass and properties of passivating layer formed in circumneutral pH conditions Collin, Marie; Fournier, Maxime; Frugier, Pierre npj Materials Degradation, Vol. 2, Issue 1 https://doi.org/10.1038/s41529-017-0025-y	journal	February 2018
A comparative review of the aqueous corrosion of glasses, crystalline ceramics, and metals Frankel, Gerald S.; Vienna, John D.; Lian, Jie npj Materials Degradation, Vol. 2, Issue 1 https://doi.org/10.1038/s41529-018-0037-2	journal	May 2018
Nanoporous silica gel structures and evolution from reactive force field-based molecular dynamics simulations Rimsza, J. M.; Du, Jincheng npj Materials Degradation, Vol. 2, Issue 1 https://doi.org/10.1038/s41529-018-0039-0	journal	July 2018
Spectroscopic ellipsometry study of thickness and porosity of the alteration layer formed on international simple glass surface in aqueous corrosion conditions Ngo, Dien; Liu, Hongshen; Sheth, Nisha npj Materials Degradation, Vol. 2, Issue 1 https://doi.org/10.1038/s41529-018-0040-7	journal	July 2018
Simplifying a solution to a complex puzzle Gin, Stéphane; Ryan, Joseph V.; Kerisit, Sébastien npj Materials Degradation, Vol. 2, Issue 1 https://doi.org/10.1038/s41529-018-0057-y	journal	November 2018
Tomographic mapping of the nanoscale water-filled pore structure in corroded borosilicate glass Perea, Daniel E.; Schreiber, Daniel K.; Ryan, Joseph V. npj Materials Degradation, Vol. 4, Issue 1 https://doi.org/10.1038/s41529-020-0110-5	journal	March 2020
Reactive simulations of the activation barrier to dissolution of amorphous silica in water Kagan, Michael; Lockwood, Glenn K.; Garofalini, Stephen H. Phys. Chem. Chem. Phys., Vol. 16, Issue 20 https://doi.org/10.1039/C4CP00030G	journal	January 2014
Molecular dynamics study of coagulation in silica-nanocolloid–water–NaCl systems based on the atomistic model Habasaki, Junko; Ishikawa, Masamichi Phys. Chem. Chem. Phys., Vol. 16, Issue 43 https://doi.org/10.1039/C4CP02984D	journal	January 2014
Hierarchically structured composites and porous materials from soft templates: fabrication and applications Thompson, Benjamin R.; Horozov, Tommy S.; Stoyanov, Simeon. D. Journal of Materials Chemistry A, Vol. 7, Issue 14 https://doi.org/10.1039/C8TA09750J	journal	January 2019
Layer analysis of the structure of water confined in vycor glass Gallo, P.; Ricci, M. A.; Rovere, M. The Journal of Chemical Physics, Vol. 116, Issue 1 https://doi.org/10.1063/1.1423662	journal	January 2002
Fractal dimensions of silica gels generated using reactive molecular dynamics simulations Bhattacharya, Sudin; Kieffer, John The Journal of Chemical Physics, Vol. 122, Issue 9 https://doi.org/10.1063/1.1857522	journal	March 2005
A molecular dynamics simulation of the vitreous silica surface Garofalini, S. H. The Journal of Chemical Physics, Vol. 78, Issue 4 https://doi.org/10.1063/1.444927	journal	February 1983
A structural analysis of the vitreous silica surface via a molecular dynamics computer simulation Levine, S. M.; Garofalini, S. H. The Journal of Chemical Physics, Vol. 86, Issue 5 https://doi.org/10.1063/1.452054	journal	March 1987
Topological and bonding defects in vitreous silica surfaces Feuston, B. P.; Garofalini, S. H. The Journal of Chemical Physics, Vol. 91, Issue 1 https://doi.org/10.1063/1.457440	journal	July 1989
New insights into the sol–gel condensation of silica by reactive molecular dynamics simulations Du, Tao; Li, Hui; Sant, Gaurav The Journal of Chemical Physics, Vol. 148, Issue 23 https://doi.org/10.1063/1.5027583	journal	June 2018
Modified Wolf electrostatic summation: Incorporating an empirical charge overlap Ma, Y.; Garofalini, S. H. Molecular Simulation, Vol. 31, Issue 11 https://doi.org/10.1080/08927020500262598	journal	September 2005
Generation of Fractal Silicas by Negative Pressure Rupturing of SiO ₂ Glass Kieffer, John; Angell, C. Austen Molecular Simulation, Vol. 3, Issue 1-3 https://doi.org/10.1080/08927028908034624	journal	May 1989
Molecular simulation of water confined in nanoporous silica Bonnaud, P. A.; Coasne, B.; Pellenq, R. J-M Journal of Physics: Condensed Matter, Vol. 22, Issue 28 https://doi.org/10.1088/0953-8984/22/28/284110	journal	June 2010
Computer simulation of local order in condensed phases of silicon Stillinger, Frank H.; Weber, Thomas A. Physical Review B, Vol. 31, Issue 8 https://doi.org/10.1103/PhysRevB.31.5262	journal	April 1985
Molecular-dynamics study of the structural correlation of porous silica with use of a parallel computer Nakano, Aiichiro; Bi, Lingsong; Kalia, Rajiv K. Physical Review B, Vol. 49, Issue 14 https://doi.org/10.1103/PhysRevB.49.9441	journal	April 1994
Structure of Random Porous Materials: Silica Aerogel Schaefer, Dale W.; Keefer, Keith D. Physical Review Letters, Vol. 56, Issue 20, p. 2199-2202 https://doi.org/10.1103/PhysRevLett.56.2199	journal	May 1986
Characterization of Ion Distributions Near the Surface of Sodium-Containing and Sodium-Depleted Calcium Aluminosilicate Melts Corrales, L. Rene; Du, Jincheng Journal of the American Ceramic Society, Vol. 89, Issue 1 https://doi.org/10.1111/j.1551-2916.2005.00695.x	journal	January 2006
Structural and Mechanical Properties of Nanoporous Silica Rimsza, J. M.; Du, Jincheng Journal of the American Ceramic Society, Vol. 97, Issue 3 https://doi.org/10.1111/jace.12707	journal	December 2013
Simulations of the surfaces of soda lime aluminoborosilicate glasses exposed to water Garofalini, Stephen H.; Ha, Ming Tai; Urraca, Joelyn Journal of the American Ceramic Society, Vol. 101, Issue 3 https://doi.org/10.1111/jace.15237	journal	October 2017
Hydration and reaction mechanisms on sodium silicate glass surfaces from molecular dynamics simulations with reactive force fields Mahadevan, Thiruvilla S.; Du, Jincheng Journal of the American Ceramic Society, Vol. 103, Issue 6 https://doi.org/10.1111/jace.17059	journal	March 2020

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