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Title: Long-term diffusion of U(VI) in bentonite: Dependence on density

Abstract

As a contribution to the safety assessment of nuclear waste repositories, U(VI) diffusion through the potential buffer material MX-80 bentonite was investigated at three clay dry densities over six years. Synthetic MX-80 model pore water was used as background electrolyte. Speciation calculations showed that Ca2UO2(CO3)3(aq) was the main U(VI) species. The in- and out-diffusion of U(VI) was investigated separately. U(VI) diffused about 3 mm, 1.5 mm, and 1 mm into the clay plug at ρ = 1.3, 1.6, and 1.9 g/cm3, respectively. No through-diffusion of the U(VI) tracer was observed. However, leaching of natural uranium contained in the clay occurred and uranium was detected in all receiving reservoirs. As expected, the effective and apparent diffusion coefficients, De and Da, decreased with increasing dry density. The Da values for the out-diffusion of natural U(VI) were in good agreement with previously determined values. Surprisingly, Da values for the in-diffusion of U(VI) were about two orders of magnitude lower than values obtained in short-term in-diffusion experiments reported in the literature. Some potential reasons for this behavior that were evaluated are changes of the U(VI) speciation within the clay (precipitation, reduction) or changes of the clay porosity and pore connectivity with time. By applyingmore » Archie's law and the extended Archie's law, it was estimated that a significantly smaller effective porosity must be present for the long-term in-diffusion of U(VI). Finally, the results suggest that long-term studies of key transport phenomena may reveal additional processes that can directly impact long-term repository safety assessments.« less

Authors:
 [1];  [2];  [3];  [4];  [4];  [1];  [1];  [1];  [1]
+ Show Author Affiliations
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Helmholtz-Zentrum Dresden-Rossendorf e.V., Dresden (Germany); Nagra, Wettingen (Switzerland)
  3. Helmholtz-Zentrum Dresden-Rossendorf e.V., Dresden (Germany); LSI Sachsen GmbH & Co., Dresden (Germany)
  4. Helmholtz-Zentrum Dresden-Rossendorf e.V., Dresden (Germany)
Publication Date:
Research Org.:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1342002
Alternate Identifier(s):
OSTI ID: 1399042
Report Number(s):
LLNL-JRNL-688984
Journal ID: ISSN 0048-9697
Grant/Contract Number:  
AC52-07NA27344; AF5865010; SCW1053
Resource Type:
Accepted Manuscript
Journal Name:
Science of the Total Environment
Additional Journal Information:
Journal Volume: 575; Journal Issue: C; Journal ID: ISSN 0048-9697
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; nuclear waste repository; MX-80; clay; uranium; speciation; extended Archie's law

Citation Formats

Joseph, Claudia, Mibus, Jens, Trepte, Paul, Muller, Christa, Brendler, Vinzenz, Park, Dan M., Jiao, Yongqin, Kersting, Annie B., and Zavarin, Mavrik. Long-term diffusion of U(VI) in bentonite: Dependence on density. United States: N. p., 2016. Web. doi:10.1016/j.scitotenv.2016.10.005.
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Joseph, Claudia, Mibus, Jens, Trepte, Paul, Muller, Christa, Brendler, Vinzenz, Park, Dan M., Jiao, Yongqin, Kersting, Annie B., & Zavarin, Mavrik. Long-term diffusion of U(VI) in bentonite: Dependence on density. United States. https://doi.org/10.1016/j.scitotenv.2016.10.005
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Joseph, Claudia, Mibus, Jens, Trepte, Paul, Muller, Christa, Brendler, Vinzenz, Park, Dan M., Jiao, Yongqin, Kersting, Annie B., and Zavarin, Mavrik. Wed . "Long-term diffusion of U(VI) in bentonite: Dependence on density". United States. https://doi.org/10.1016/j.scitotenv.2016.10.005. https://www.osti.gov/servlets/purl/1342002.
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@article{osti_1342002,
title = {Long-term diffusion of U(VI) in bentonite: Dependence on density},
author = {Joseph, Claudia and Mibus, Jens and Trepte, Paul and Muller, Christa and Brendler, Vinzenz and Park, Dan M. and Jiao, Yongqin and Kersting, Annie B. and Zavarin, Mavrik},
abstractNote = {As a contribution to the safety assessment of nuclear waste repositories, U(VI) diffusion through the potential buffer material MX-80 bentonite was investigated at three clay dry densities over six years. Synthetic MX-80 model pore water was used as background electrolyte. Speciation calculations showed that Ca2UO2(CO3)3(aq) was the main U(VI) species. The in- and out-diffusion of U(VI) was investigated separately. U(VI) diffused about 3 mm, 1.5 mm, and 1 mm into the clay plug at ρ = 1.3, 1.6, and 1.9 g/cm3, respectively. No through-diffusion of the U(VI) tracer was observed. However, leaching of natural uranium contained in the clay occurred and uranium was detected in all receiving reservoirs. As expected, the effective and apparent diffusion coefficients, De and Da, decreased with increasing dry density. The Da values for the out-diffusion of natural U(VI) were in good agreement with previously determined values. Surprisingly, Da values for the in-diffusion of U(VI) were about two orders of magnitude lower than values obtained in short-term in-diffusion experiments reported in the literature. Some potential reasons for this behavior that were evaluated are changes of the U(VI) speciation within the clay (precipitation, reduction) or changes of the clay porosity and pore connectivity with time. By applying Archie's law and the extended Archie's law, it was estimated that a significantly smaller effective porosity must be present for the long-term in-diffusion of U(VI). Finally, the results suggest that long-term studies of key transport phenomena may reveal additional processes that can directly impact long-term repository safety assessments.},
doi = {10.1016/j.scitotenv.2016.10.005},
journal = {Science of the Total Environment},
number = C,
volume = 575,
place = {United States},
year = {Wed Oct 12 00:00:00 EDT 2016},
month = {Wed Oct 12 00:00:00 EDT 2016}
}
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https://doi.org/10.1016/j.scitotenv.2016.10.005
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