skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Structural role of ZrO2 and its impact on properties of boroaluminosilicate nuclear waste glasses

Abstract

Addition of zirconia (ZrO2) to nuclear waste glasses, even in small amount, significantly affects physical properties such as chemical durability, density, viscosity, and glass transition temperature. Hence ZrO2 plays an important role in the development of nuclear waste glass compositions. It was found recently that addition of zirconia decreases the initial dissolution rate but increases long-term dissolution by changing the protective properties such as porosity of alteration layers. In this study, the International Simple Glass (ISG) with different amounts of ZrO2/SiO2 substitution was simulated using classical molecular dynamics (MD) simulations and recently developed composition-dependent potential sets. Local structural descriptors such as bond distances, bond angle distributions, and coordination numbers were systematically studied and compared with experimental values. Zr K-edge extended X-ray absorption fine structure spectra were also calculated and compared with experiment to resolve the local coordination environment around Zr. Medium-range structural information (e.g., Qn distribution, network connectivity, and ring-size distribution) showed that ZrO2/SiO2 substitution increases the overall network connectivity and the amount of smaller sized rings, which will decrease the initial dissolution rate by strengthening the glass network and limiting water diffusivity. Finally, diffusion and dynamic properties of the ions were studied and discussed to develop a better understandingmore » of the chemical durability of these glasses.« less

Authors:
 [1];  [1];  [2]; ORCiD logo [1]
  1. Univ. of North Texas, Denton, TX (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Performance and Design of Nuclear Waste Forms and Containers (WastePD); Univ. of North Texas, Denton, TX (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1668035
Grant/Contract Number:  
SC0016584
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
npj Materials Degradation
Additional Journal Information:
Journal Volume: 2; Journal Issue: 1; Journal ID: ISSN 2397-2106
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Lu, Xiaonan, Deng, Lu, Kerisit, Sebastien, and Du, Jincheng. Structural role of ZrO2 and its impact on properties of boroaluminosilicate nuclear waste glasses. United States: N. p., 2018. Web. doi:10.1038/s41529-018-0041-6.
Lu, Xiaonan, Deng, Lu, Kerisit, Sebastien, & Du, Jincheng. Structural role of ZrO2 and its impact on properties of boroaluminosilicate nuclear waste glasses. United States. https://doi.org/10.1038/s41529-018-0041-6
Lu, Xiaonan, Deng, Lu, Kerisit, Sebastien, and Du, Jincheng. 2018. "Structural role of ZrO2 and its impact on properties of boroaluminosilicate nuclear waste glasses". United States. https://doi.org/10.1038/s41529-018-0041-6. https://www.osti.gov/servlets/purl/1668035.
@article{osti_1668035,
title = {Structural role of ZrO2 and its impact on properties of boroaluminosilicate nuclear waste glasses},
author = {Lu, Xiaonan and Deng, Lu and Kerisit, Sebastien and Du, Jincheng},
abstractNote = {Addition of zirconia (ZrO2) to nuclear waste glasses, even in small amount, significantly affects physical properties such as chemical durability, density, viscosity, and glass transition temperature. Hence ZrO2 plays an important role in the development of nuclear waste glass compositions. It was found recently that addition of zirconia decreases the initial dissolution rate but increases long-term dissolution by changing the protective properties such as porosity of alteration layers. In this study, the International Simple Glass (ISG) with different amounts of ZrO2/SiO2 substitution was simulated using classical molecular dynamics (MD) simulations and recently developed composition-dependent potential sets. Local structural descriptors such as bond distances, bond angle distributions, and coordination numbers were systematically studied and compared with experimental values. Zr K-edge extended X-ray absorption fine structure spectra were also calculated and compared with experiment to resolve the local coordination environment around Zr. Medium-range structural information (e.g., Qn distribution, network connectivity, and ring-size distribution) showed that ZrO2/SiO2 substitution increases the overall network connectivity and the amount of smaller sized rings, which will decrease the initial dissolution rate by strengthening the glass network and limiting water diffusivity. Finally, diffusion and dynamic properties of the ions were studied and discussed to develop a better understanding of the chemical durability of these glasses.},
doi = {10.1038/s41529-018-0041-6},
url = {https://www.osti.gov/biblio/1668035}, journal = {npj Materials Degradation},
issn = {2397-2106},
number = 1,
volume = 2,
place = {United States},
year = {Fri Jun 22 00:00:00 EDT 2018},
month = {Fri Jun 22 00:00:00 EDT 2018}
}

Works referenced in this record:

The structural role of Zr within alkali borosilicate glasses for nuclear waste immobilisation
journal, April 2011


Origin and consequences of silicate glass passivation by surface layers
journal, February 2015


X-ray absorption studies of the local environment of Zr in high-zirconia borosilicate glasses
journal, November 1999


Wet Chemical and UV-Vis Spectrometric Iron Speciation in Quenched Low and Intermediate Level Nuclear Waste Glasses
journal, January 2015


First-Principles Study of Hydrolysis Reaction Barriers in a Sodium Borosilicate Glass
journal, November 2013


A Preliminary Investigation of the ISG Glass Vapor Hydration
journal, October 2013


The Structural Properties of Cations in Nuclear Glasses
journal, January 2014


Boron Speciation in Soda-Lime Borosilicate Glasses Containing Zirconium: Boron Speciation in Soda-Lime Borosilicate Glasses
journal, April 2010


Structure, dynamics, and electronic properties of lithium disilicate melt and glass
journal, September 2006


Predicting the bioactivity of glasses using the network connectivity or split network models
journal, December 2011


Oxide glass structure evolution under swift heavy ion irradiation
journal, April 2014


Europium environment and clustering in europium doped silica and sodium silicate glasses
journal, June 2011


An international initiative on long-term behavior of high-level nuclear waste glass
journal, June 2013


First investigations of the influence of IVB elements (Ti, Zr, and Hf) on the chemical durability of soda-lime borosilicate glasses
journal, October 2010


Evidence for 6-Coordinated Zirconium in Inactive Nuclear Waste Glasses
journal, August 1999


A Neutron and X-Ray Diffraction Study of Bioglass® with Reverse Monte Carlo Modelling
journal, December 2007


Mechanisms of boron coordination change between borosilicate glasses and melts
journal, November 2013


Parameter-free calculations of X-ray spectra with FEFF9
journal, January 2010


Evidence for symmetric cationic sites in zirconium-bearing oxide glasses
journal, June 2006


Raman Response of Network Modifier Cations in Alumino-Silicate Glasses
journal, February 2015


Ab initio theory and calculations of X-ray spectra
journal, July 2009


Global Model for Calculating Room-Temperature Glass Density from the Composition
journal, August 2007


Determination of the Forward Dissolution Rate for International Simple Glass in Alkaline Solutions
journal, January 2017


Quantitative morphological and compositional evaluation of laboratory prepared aluminoborosilicate glass surfaces
journal, January 2015


Soda lime zirconia silicate glasses as prospective hosts for zirconia-containing radioactive wastes
journal, April 2005


Effect of Strontium Substitution on the Structure of 45S5 Bioglasses
journal, June 2011


Structural insights for the International Simple Glass by combining X-ray absorption spectroscopic analysis and atomistic modelling
journal, November 2018


Why Do Certain Glasses with a High Dissolution Rate Undergo a Low Degree of Corrosion?
journal, March 2011


The use of positrons to survey alteration layers on synthetic nuclear waste glasses
journal, July 2017


Structure and properties of sodium aluminosilicate glasses from molecular dynamics simulations
journal, July 2013


Glass Corrosion in the Presence of Iron-Bearing Materials and Potential Corrosion Suppressors
journal, January 2015


Insight into silicate-glass corrosion mechanisms
journal, October 2008


Micro-channel as a New Tool to Investigate Glass Dissolution Kinetics
journal, January 2014


Rare earth ion clustering behavior in europium doped silicate glasses: Simulation size and glass structure effect
journal, December 2012


Effects of boron oxide substitution on the structure and bioactivity of SrO-containing bioactive glasses
journal, February 2017


Structural Origin of the Thermal and Diffusion Behaviors of Lithium Aluminosilicate Crystal Polymorphs and Glasses
journal, May 2016


An enhanced resolution of the structural environment of zirconium in borosilicate glasses
journal, December 2013


Molecular dynamics simulation of radiation damage in glasses
journal, July 2011


Liquidus temperature and chemical durability of selected glasses to immobilize rare earth oxides waste
journal, October 2015


The effect of molecular structure on borosilicate glass leaching
journal, October 1986


The structure of erbium doped sodium silicate glasses
journal, August 2005


Structure–property relationships in multicomponent oxide glasses
journal, December 2002


Lithium vanado-phosphate glasses: Structure and dynamics properties studied by molecular dynamics simulations
journal, November 2014


Formulation, Testing, and Structural Characterization of High-Zirconium High-Level Waste Glasses
journal, January 1999


Molecular dynamics simulations of soda–lime–silicate glasses
journal, November 2001


Short- and medium-range structure of amorphous zircon from molecular dynamics simulations
journal, December 2006


Alpha Decays Impact on Nuclear Glass Structure
journal, January 2014


Durability of GFRP bars: a critical review of the literature
journal, January 2005


Initial Dissolution Rate of the International Simple Glass as a Function of pH and Temperature Measured Using Microchannel Flow-Through Test Method
journal, October 2013


The medium range structure of sodium silicate glasses: a molecular dynamics simulation
journal, December 2004


The fate of silicon during glass corrosion under alkaline conditions: A mechanistic and kinetic study with the International Simple Glass
journal, February 2015


New Insight into the Residual Rate of Borosilicate Glasses: Effect of S/V and Glass Composition
journal, October 2013


Structure of International Simple Glass and properties of passivating layer formed in circumneutral pH conditions
journal, February 2018


The Structure of Bioactive Silicate Glasses:  New Insight from Molecular Dynamics Simulations
journal, January 2007


Structure study of multi-component borosilicate glasses from high-Q neutron diffraction measurement and RMC modeling
journal, June 2008


Resumption of nuclear glass alteration: State of the art
journal, May 2014


Theoretical approaches to x-ray absorption fine structure
journal, July 2000


IFEFFIT  : interactive XAFS analysis and FEFF fitting
journal, March 2001


Short- and medium-range structures of cerium aluminophosphate glasses: A molecular dynamics study
journal, November 2014


Self-healing capacity of nuclear glass observed by NMR spectroscopy
journal, May 2016


Differential anomalous wide-angle X-ray scattering and X-ray absorption experiments to investigate the formation of glass ceramics in the CaO–SiO 2 –ZrO 2 system
journal, December 1999


Magnetosomes could be protective shields against metal stress in magnetotactic bacteria
journal, July 2020


Works referencing / citing this record:

Simplifying a solution to a complex puzzle
journal, November 2018


Development of boron oxide potentials for computer simulations of multicomponent oxide glasses
journal, October 2018


Interfacial structures of spinel crystals with borosilicate nuclear waste glasses from molecular dynamics simulations
journal, February 2019