Colloid-facilitated transport of 238Pu, 233U and 137Cs through fractured chalk: Laboratory experiments, modelling, and implications for nuclear waste disposal

Tran, Emily; Zavrin, Mavrik; Kersting, Annie B.; Klein-BenDavid, Ofra; Teutsch, Nadya; Weisbrod, Noam

doi:10.1016/j.scitotenv.2020.143818

Title: Colloid-facilitated transport of ²³⁸Pu, ²³³U and ¹³⁷Cs through fractured chalk: Laboratory experiments, modelling, and implications for nuclear waste disposal

Journal Article · Thu Nov 19 00:00:00 EST 2020 · Science of the Total Environment

DOI:https://doi.org/10.1016/j.scitotenv.2020.143818· OSTI ID:1734598

Tran, Emily ^[1]; Zavrin, Mavrik ^[2]; Kersting, Annie B. ^[2]; Klein-BenDavid, Ofra ^[3]; Teutsch, Nadya ^[4]; Weisbrod, Noam ^[1]

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)

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 (K_d, 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 K_d = 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 K_d = 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.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); Israeli Atomic Energy Agency; Israel Science Foundation

Grant/Contract Number:: AC52-07NA27344; 287/17; 165/17

OSTI ID:: 1734598

Alternate ID(s):: OSTI ID: 1818529

Report Number(s):: LLNL-JRNL-814044; 1021970; TRN: US2205174

Journal Information:: Science of the Total Environment, Vol. 757, Issue C; ISSN 0048-9697

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Colloid-facilitated transport of ²³⁸Pu, ²³³U and ¹³⁷Cs through fractured chalk: Laboratory experiments, modelling, and implications for nuclear waste disposal