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Title: Accelerated Leach Testing of Glass (ALTGLASS): II. Mineralization of hydrogels by leachate strong bases

The durability of high level nuclear waste glasses must be predicted on geological time scales. Waste glass surfaces form hydrogels when in contact with water for varying test durations. As the glass hydrogels age, some exhibit an undesirable resumption of dissolution at long times while others exhibit near steady-state dissolution, that is, nonresumption of dissolution. Resumption of dissolution is associated with the formation of zeolitic phases while nonresumption of dissolution is associated with the formation of clay minerals. Hydrogels with a stoichiometry close to that of imogolite, (Al 2O 3·Si(OH) 4), with ferrihydrite (Fe 2O 3·0.5H 2O), have been shown to be associated with waste glasses that resume dissolution. Aluminosilicate hydrogels with a stoichiometry of allophane-hisingerite ((Al,Fe) 2O 3·1.3-2Si(OH) 4) have been shown to be associated with waste glasses that exhibit near steady-state dissolution at long times. These phases are all amorphous and poorly crystalline and are also found on natural weathered basalt glasses. Interaction of these hydrogels with excess alkali and OH (strong base) in the leachates, causes the Al 2O 3· nSiO 2 (where n=1-2) hydrogels to mineralize to zeolites. Excess alkali in the leachate is generated by alkali in the glass. As a result, preliminary rate-determiningmore » leach layer forming exchange reactions are hypothesized based on these findings.« less
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1]
  1. Savannah River National Lab., Aiken, SC (United States)
Publication Date:
Report Number(s):
SRNL-STI-2014-00381
Journal ID: ISSN 2041-1286
Grant/Contract Number:
AC09-08SR22470
Type:
Accepted Manuscript
Journal Name:
International Journal of Applied Glass Science
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1286
Publisher:
American Ceramic Society
Research Org:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 36 MATERIALS SCIENCE; corrosion; glass durability; glass leaching; modeling; nuclear waste; aging
OSTI Identifier:
1372632

Jantzen, Carol M., Trivelpiece, Cory L., Crawford, Charles L., Pareizs, John M., and Pickett, John B.. Accelerated Leach Testing of Glass (ALTGLASS): II. Mineralization of hydrogels by leachate strong bases. United States: N. p., Web. doi:10.1111/ijag.12264.
Jantzen, Carol M., Trivelpiece, Cory L., Crawford, Charles L., Pareizs, John M., & Pickett, John B.. Accelerated Leach Testing of Glass (ALTGLASS): II. Mineralization of hydrogels by leachate strong bases. United States. doi:10.1111/ijag.12264.
Jantzen, Carol M., Trivelpiece, Cory L., Crawford, Charles L., Pareizs, John M., and Pickett, John B.. 2017. "Accelerated Leach Testing of Glass (ALTGLASS): II. Mineralization of hydrogels by leachate strong bases". United States. doi:10.1111/ijag.12264. https://www.osti.gov/servlets/purl/1372632.
@article{osti_1372632,
title = {Accelerated Leach Testing of Glass (ALTGLASS): II. Mineralization of hydrogels by leachate strong bases},
author = {Jantzen, Carol M. and Trivelpiece, Cory L. and Crawford, Charles L. and Pareizs, John M. and Pickett, John B.},
abstractNote = {The durability of high level nuclear waste glasses must be predicted on geological time scales. Waste glass surfaces form hydrogels when in contact with water for varying test durations. As the glass hydrogels age, some exhibit an undesirable resumption of dissolution at long times while others exhibit near steady-state dissolution, that is, nonresumption of dissolution. Resumption of dissolution is associated with the formation of zeolitic phases while nonresumption of dissolution is associated with the formation of clay minerals. Hydrogels with a stoichiometry close to that of imogolite, (Al2O3·Si(OH)4), with ferrihydrite (Fe2O3·0.5H2O), have been shown to be associated with waste glasses that resume dissolution. Aluminosilicate hydrogels with a stoichiometry of allophane-hisingerite ((Al,Fe)2O3·1.3-2Si(OH)4) have been shown to be associated with waste glasses that exhibit near steady-state dissolution at long times. These phases are all amorphous and poorly crystalline and are also found on natural weathered basalt glasses. Interaction of these hydrogels with excess alkali and OH– (strong base) in the leachates, causes the Al2O3·nSiO2 (where n=1-2) hydrogels to mineralize to zeolites. Excess alkali in the leachate is generated by alkali in the glass. As a result, preliminary rate-determining leach layer forming exchange reactions are hypothesized based on these findings.},
doi = {10.1111/ijag.12264},
journal = {International Journal of Applied Glass Science},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {2}
}