Selenium interaction with iron minerals: Quantitative comparison of sorption and coprecipitation impacts on mobility

Balboni, Enrica; Han, Sol-chan; Zavarin, Mavrik

doi:10.1016/j.apgeochem.2024.106194

Title: Selenium interaction with iron minerals: Quantitative comparison of sorption and coprecipitation impacts on mobility

Journal Article · 10 October 2024 · Applied Geochemistry

DOI: https://doi.org/10.1016/j.apgeochem.2024.106194 · OSTI ID:2478208

^[1]; Han, Sol-chan ^[2]; Zavarin, Mavrik ^[1]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Given the significance of selenium (Se) as a micronutrient, the radioactive nature of some of its isotopes, and its affinity to iron (Fe) minerals, extensive research has been conducted on the sorption mechanisms between Se and these minerals. Here, in this study, we employ sorption data sourced from the L-SCIE database and coprecipitation data from available literature to achieve the following objectives: i) establish coherence between adsorption and coprecipitation processes, ii) quantitatively evaluate the importance of these processes in nuclear waste repository science, and iii) propose a forward-looking approach for integrating coprecipitation into reactive transport models. Our findings indicate that a correlation between Se adsorption and coprecipitation can be established using the λ formalism. The comparable log(λ_Se(IV)/λ_Se(VI)) ratios derived from adsorption and coprecipitation experiments suggest that these processes can be quantitatively compared and evaluated using our numerical approach. Across all iron oxide phases examined, coprecipitation leads to significantly greater immobilization of Se compared to adsorption. Specifically, for hydrous ferric oxide, hematite, and goethite, coprecipitation is predicted to result in 100–1000 times more Se immobilization compared to adsorption, irrespective of the Se oxidation state (Se(IV) or Se(VI)); notably stronger immobilization potential via coprecipitation was observed for magnetite. The modeling approach and quantitative analysis presented herein clearly highlight the importance of including coprecipitation processes when simulating Se (and other elements) transport, particularly under conditions where mineral compositions are transient or evolving with time. Neglecting coprecipitation in models is likely to lead to significant overestimates of migration.

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

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Nuclear Energy (NE), Office of Spent Fuel and Waste Disposition. Office of Spent Fuel and Waste Science and Technology

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 2478208

Report Number(s):: LLNL--JRNL-861948; 1093207

Journal Information:: Applied Geochemistry, Journal Name: Applied Geochemistry Vol. 175; ISSN 0883-2927

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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