Colloid-facilitated transport of 238Pu, 233U and 137Cs through fractured chalk: Laboratory experiments, modelling, and implications for nuclear waste disposal
Abstract
The influence of montmorillonite colloids on the mobility of 238Pu, 233U and 137Cs through a chalk fracture was investigated to assess the transport potential for radioactive waste. Radioisotopes of each element, along with the conservative tracer tritium, were injected in the presence and absence of montmorillonite colloids into a naturally fractured chalk core. In parallel, batch experiments were conducted to obtain experimental sorption coefficients (Kd, mL/g) for both montmorillonite colloids and the chalk fracture material. Breakthrough curves were modelled to determine diffusivity and sorption of each radionuclide to the chalk and the colloids under advective conditions. Uranium sorbed sparingly to chalk (log Kd = 0.7 ± 0.2) in batch sorption experiments. 233U(VI) breakthrough was controlled primarily by the matrix diffusion and sorption to chalk (15 and 25% recovery with and without colloids, respectively). Cesium, in contrast, sorbed strongly to both the montmorillonite colloids and chalk (batch log Kd = 3.2 ± 0.01 and 3.9 ± 0.01, respectively). The high affinity to chalk and low colloid concentrations overwhelmed any colloidal Cs transport, resulting in very low 137Cs breakthrough (1.1–5.5% mass recovery). Batch and fracture transport results, and the associated modelling revealed that Pu migrates both as Pu (IV) sorbed to montmorillonitemore »
- Authors:
-
- Ben Gurlon Univ. of the Negev, Midreshet Ben Gurion (Israel)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Nuclear Research Center of the Negev, Beersheva (Israel); Ben Gurion Univ. of the Negev, Beersheva (Israel)
- Geological Survey of Israel, Jerusalem (Israel)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); Israeli Atomic Energy Agency; Israel Science Foundation
- OSTI Identifier:
- 1734598
- Alternate Identifier(s):
- OSTI ID: 1818529
- Report Number(s):
- LLNL-JRNL-814044
Journal ID: ISSN 0048-9697; 1021970; TRN: US2205174
- Grant/Contract Number:
- AC52-07NA27344; 287/17; 165/17
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science of the Total Environment
- Additional Journal Information:
- Journal Volume: 757; Journal Issue: C; Journal ID: ISSN 0048-9697
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; radiation chemistry; radiochemistry; nuclear chemistry; radionuclides; montmorillonite colloids; carbonate rocks; reactive transport
Citation Formats
Tran, Emily, Zavrin, Mavrik, Kersting, Annie B., Klein-BenDavid, Ofra, Teutsch, Nadya, and Weisbrod, Noam. Colloid-facilitated transport of 238Pu, 233U and 137Cs through fractured chalk: Laboratory experiments, modelling, and implications for nuclear waste disposal. United States: N. p., 2020.
Web. doi:10.1016/j.scitotenv.2020.143818.
Tran, Emily, Zavrin, Mavrik, Kersting, Annie B., Klein-BenDavid, Ofra, Teutsch, Nadya, & Weisbrod, Noam. Colloid-facilitated transport of 238Pu, 233U and 137Cs through fractured chalk: Laboratory experiments, modelling, and implications for nuclear waste disposal. United States. https://doi.org/10.1016/j.scitotenv.2020.143818
Tran, Emily, Zavrin, Mavrik, Kersting, Annie B., Klein-BenDavid, Ofra, Teutsch, Nadya, and Weisbrod, Noam. Thu .
"Colloid-facilitated transport of 238Pu, 233U and 137Cs through fractured chalk: Laboratory experiments, modelling, and implications for nuclear waste disposal". United States. https://doi.org/10.1016/j.scitotenv.2020.143818. https://www.osti.gov/servlets/purl/1734598.
@article{osti_1734598,
title = {Colloid-facilitated transport of 238Pu, 233U and 137Cs through fractured chalk: Laboratory experiments, modelling, and implications for nuclear waste disposal},
author = {Tran, Emily and Zavrin, Mavrik and Kersting, Annie B. and Klein-BenDavid, Ofra and Teutsch, Nadya and Weisbrod, Noam},
abstractNote = {The influence of montmorillonite colloids on the mobility of 238Pu, 233U and 137Cs through a chalk fracture was investigated to assess the transport potential for radioactive waste. Radioisotopes of each element, along with the conservative tracer tritium, were injected in the presence and absence of montmorillonite colloids into a naturally fractured chalk core. In parallel, batch experiments were conducted to obtain experimental sorption coefficients (Kd, mL/g) for both montmorillonite colloids and the chalk fracture material. Breakthrough curves were modelled to determine diffusivity and sorption of each radionuclide to the chalk and the colloids under advective conditions. Uranium sorbed sparingly to chalk (log Kd = 0.7 ± 0.2) in batch sorption experiments. 233U(VI) breakthrough was controlled primarily by the matrix diffusion and sorption to chalk (15 and 25% recovery with and without colloids, respectively). Cesium, in contrast, sorbed strongly to both the montmorillonite colloids and chalk (batch log Kd = 3.2 ± 0.01 and 3.9 ± 0.01, respectively). The high affinity to chalk and low colloid concentrations overwhelmed any colloidal Cs transport, resulting in very low 137Cs breakthrough (1.1–5.5% mass recovery). Batch and fracture transport results, and the associated modelling revealed that Pu migrates both as Pu (IV) sorbed to montmorillonite colloids and as dissolved Pu(V) (7% recovery). Transport experiments revealed differences in Pu(IV) and Pu(V) transport behavior that could not be quantified in simple batch experiments but are critical to effectively predict transport behavior of redox-sensitive radionuclides. Finally, a brackish groundwater solution was injected after completion of the fracture flow experiments and resulted in remobilization and recovery of 2.2% of the total sorbed radionuclides which remained in the core from previous experiments. In general, our study demonstrates consistency in sorption behavior between batch and advective fracture transport. Finally, the results suggest that colloid-facilitated radionuclide transport will enhance radionuclide migration in fractured chalk for those radionuclides with exceedingly high affinity for colloids.},
doi = {10.1016/j.scitotenv.2020.143818},
journal = {Science of the Total Environment},
number = C,
volume = 757,
place = {United States},
year = {Thu Nov 19 00:00:00 EST 2020},
month = {Thu Nov 19 00:00:00 EST 2020}
}
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