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Title: On the long-term migration of uranyl in bentonite barrier for high-level radioactive waste repositories: The effect of different host rocks

Abstract

Repositories for high level radioactive waste hosted in argillite or granite with bentonite backfill are the two disposal concepts that been extensively studied. A general perception is that granite has very low sorption capacity and therefore is disadvantageous in retarding the migration of radionuclides in comparison with argillite. However, when there is bentonite backfill, does the sorption capacity of granite really matter for the migration of radionuclides? How different host rocks would affect the migration of U(VI) through the bentonite backfill of an engineered barrier system (EBS), and which properties of the host rocks cause those differences in migration, given that migration of radionuclides is a critical measure in assessing the performance of a repository? Here we present two coupled thermal, hydrological, and chemical models for the transport of U(VI), each with an identical setup except for the type of host rock (argillite vs granite rock). Comparisons between our models show that the different host rocks exert their influence on migration of U(VI) via regulating the chemical conditions in the bentonite, which affect the concentration of U(VI) at the source and the adsorption of U(VI) in the bentonite. The key chemical conditions are pH, Ca+, and HCO3- concentration in pore-water,more » which are strongly affected by soluble carbonate minerals. Our models also show the occurrence of illitization (dissolution of smectite and precipitation of illite) in the bentonite, which affects the migration of U(VI) through changing pH and the quantity of adsorbents. Although generalization of current model results for granite and argillite should be done carefully, the simulations highlight the importance of pore-water chemistry in host rock, as well as bentonite-host rock interactions, when assessing the performance of a repository. In comparison to properties such as thermal conductivity, permeability, and adsorption capacity, properties that have been studied intensively, the pore-water chemistry of host rocks deserve equal or even more attention because of its strong influence on radionuclide migration.« less

Authors:
 [1];  [2];  [1];  [3]
+ Show Author Affiliations
  1. Tsinghua Univ., Beijing (China). School of Environment
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Geosciences Division
  3. Beijing Normal Univ., Beijing (China). College of Water Sciences
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1559249
Alternate Identifier(s):
OSTI ID: 1543182
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Geology
Additional Journal Information:
Journal Volume: 525; Journal Issue: C; Journal ID: ISSN 0009-2541
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES

Citation Formats

Cao, Xiaoyuan, Zheng, Liange, Hou, Deyi, and Hu, Litang. On the long-term migration of uranyl in bentonite barrier for high-level radioactive waste repositories: The effect of different host rocks. United States: N. p., 2019. Web. doi:10.1016/j.chemgeo.2019.07.006.
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Cao, Xiaoyuan, Zheng, Liange, Hou, Deyi, & Hu, Litang. On the long-term migration of uranyl in bentonite barrier for high-level radioactive waste repositories: The effect of different host rocks. United States. https://doi.org/10.1016/j.chemgeo.2019.07.006
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Cao, Xiaoyuan, Zheng, Liange, Hou, Deyi, and Hu, Litang. Thu . "On the long-term migration of uranyl in bentonite barrier for high-level radioactive waste repositories: The effect of different host rocks". United States. https://doi.org/10.1016/j.chemgeo.2019.07.006. https://www.osti.gov/servlets/purl/1559249.
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@article{osti_1559249,
title = {On the long-term migration of uranyl in bentonite barrier for high-level radioactive waste repositories: The effect of different host rocks},
author = {Cao, Xiaoyuan and Zheng, Liange and Hou, Deyi and Hu, Litang},
abstractNote = {Repositories for high level radioactive waste hosted in argillite or granite with bentonite backfill are the two disposal concepts that been extensively studied. A general perception is that granite has very low sorption capacity and therefore is disadvantageous in retarding the migration of radionuclides in comparison with argillite. However, when there is bentonite backfill, does the sorption capacity of granite really matter for the migration of radionuclides? How different host rocks would affect the migration of U(VI) through the bentonite backfill of an engineered barrier system (EBS), and which properties of the host rocks cause those differences in migration, given that migration of radionuclides is a critical measure in assessing the performance of a repository? Here we present two coupled thermal, hydrological, and chemical models for the transport of U(VI), each with an identical setup except for the type of host rock (argillite vs granite rock). Comparisons between our models show that the different host rocks exert their influence on migration of U(VI) via regulating the chemical conditions in the bentonite, which affect the concentration of U(VI) at the source and the adsorption of U(VI) in the bentonite. The key chemical conditions are pH, Ca+, and HCO3- concentration in pore-water, which are strongly affected by soluble carbonate minerals. Our models also show the occurrence of illitization (dissolution of smectite and precipitation of illite) in the bentonite, which affects the migration of U(VI) through changing pH and the quantity of adsorbents. Although generalization of current model results for granite and argillite should be done carefully, the simulations highlight the importance of pore-water chemistry in host rock, as well as bentonite-host rock interactions, when assessing the performance of a repository. In comparison to properties such as thermal conductivity, permeability, and adsorption capacity, properties that have been studied intensively, the pore-water chemistry of host rocks deserve equal or even more attention because of its strong influence on radionuclide migration.},
doi = {10.1016/j.chemgeo.2019.07.006},
journal = {Chemical Geology},
number = C,
volume = 525,
place = {United States},
year = {Thu Jul 04 00:00:00 EDT 2019},
month = {Thu Jul 04 00:00:00 EDT 2019}
}
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https://doi.org/10.1016/j.chemgeo.2019.07.006
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Figures / Tables:

Table 1 Table 1: The surface protonation reactions on montmorillonite (smectite) and illite and surface complexation reactions for the sorption of U(VI) on montmorillonite (smectite) and illite
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