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Title: Corrosion of the International Simple Glass under acidic to hyperalkaline conditions

Abstract

Assessment of glass dissolution kinetics, under disposal relevant temperature and pH environments, is required to credibly estimate radionuclide release rates from vitrified radioactive waste. Leaching of the International Simple Glass (ISG) under acidic to hyperalkaline conditions was examined. Forward rate measurements have been obtained using the dynamic leaching SPFT protocol and rate parameters for B, Na and Si in the basic regime; errors in rates predicted using these parameters at high pH and temperature are significant because the fitting uses logarithmic data. Longer term behaviour under hyperalkaline conditions, representative of some disposal environments, was investigated using the PCT and MCC-1 static leaching protocols with Ca(OH)2 solutions for up to 120 days (PCT) and 720 days (MCC-1). In hyperalkaline conditions dissolution was incongruent for all elements and the presence of alternating zirconia-rich and zirconia-poor alteration layers was viewed on all leached monoliths, indicating the occurrence of a self-organisation phenomenon during leaching.

Authors:
 [1];  [1]; ORCiD logo [2]; ORCiD logo [1];  [1]; ORCiD logo [1]
  1. Univ. of Sheffield (United Kingdom)
  2. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1513249
Report Number(s):
PNNL-SA-139241
Journal ID: ISSN 2397-2106
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
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

Backhouse, Daniel J., Fisher, Adam J., Neeway, James J., Corkhill, Claire L., Hyatt, Neil C., and Hand, Russell J. Corrosion of the International Simple Glass under acidic to hyperalkaline conditions. United States: N. p., 2018. Web. doi:10.1038/s41529-018-0050-5.
Backhouse, Daniel J., Fisher, Adam J., Neeway, James J., Corkhill, Claire L., Hyatt, Neil C., & Hand, Russell J. Corrosion of the International Simple Glass under acidic to hyperalkaline conditions. United States. https://doi.org/10.1038/s41529-018-0050-5
Backhouse, Daniel J., Fisher, Adam J., Neeway, James J., Corkhill, Claire L., Hyatt, Neil C., and Hand, Russell J. Mon . "Corrosion of the International Simple Glass under acidic to hyperalkaline conditions". United States. https://doi.org/10.1038/s41529-018-0050-5. https://www.osti.gov/servlets/purl/1513249.
@article{osti_1513249,
title = {Corrosion of the International Simple Glass under acidic to hyperalkaline conditions},
author = {Backhouse, Daniel J. and Fisher, Adam J. and Neeway, James J. and Corkhill, Claire L. and Hyatt, Neil C. and Hand, Russell J.},
abstractNote = {Assessment of glass dissolution kinetics, under disposal relevant temperature and pH environments, is required to credibly estimate radionuclide release rates from vitrified radioactive waste. Leaching of the International Simple Glass (ISG) under acidic to hyperalkaline conditions was examined. Forward rate measurements have been obtained using the dynamic leaching SPFT protocol and rate parameters for B, Na and Si in the basic regime; errors in rates predicted using these parameters at high pH and temperature are significant because the fitting uses logarithmic data. Longer term behaviour under hyperalkaline conditions, representative of some disposal environments, was investigated using the PCT and MCC-1 static leaching protocols with Ca(OH)2 solutions for up to 120 days (PCT) and 720 days (MCC-1). In hyperalkaline conditions dissolution was incongruent for all elements and the presence of alternating zirconia-rich and zirconia-poor alteration layers was viewed on all leached monoliths, indicating the occurrence of a self-organisation phenomenon during leaching.},
doi = {10.1038/s41529-018-0050-5},
journal = {npj Materials Degradation},
number = 1,
volume = 2,
place = {United States},
year = {Mon Sep 10 00:00:00 EDT 2018},
month = {Mon Sep 10 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Fig. 1 Fig. 1: a B & Si dissolution rates (g m–2 d–1) versus log10[($q$/$S$)/(m s–1)] where $q$ is flow-rate and $S$ is sample-surface-area at pH(RT) 9 and 40 °C determined from SPFT showing data from this study and Neeway et al. Error bars are the standard error calculated using Eqs. (7)–(8);more » b Compiled forward dissolution rates using data from this study and from Neeway et al. showing log10 [RB/(g m –2 d–1)] versus pH (modelled at experimental temperature) from all experiments. The solid lines are obtained from a multiple linear regression fit to the data in the basic regime (pH 8–12) whereas dashed lines in the acidic regime are a guide to the eye. Error bars are the standard error calculated using Eqs. (7)– (8); c Si forward rate data compared to other studies; d, e particles after 100 days SPFT at pH(RT) 11, 40 °C & log10[($q$/$S$)/(m s–1)] = –6.81, features A in (d) are indicative of localised preferential attack; features B in (e) appear to be dehydration cracks« less

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.