Organic Complexation of U(VI) in Reducing Soils at a Natural Analogue Site: Implications for Uranium Transport

Adam J. Fuller, Peter Leary, Neil D. Gray, Helena S. Davies, J. Frederick W. Mosselmans, Filipa Cox, Clare H. Robinson, Jon K. Pittman, Clare M. McCann, Michael Muir, Margaret C. Graham, Satoshi Utsunomiya, William R. Bower, Katherine Morris, Samuel Shaw, Pieter Bots, Francis R. Livens, Gareth T. W. Law

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Sammanfattning

Understanding the long-term fate, stability, and bioavailability of uranium (U) in the environment is important for the management of nuclear legacy sites and radioactive wastes. Analysis of U behavior at natural analogue sites permits evaluation of U biogeochemistry under conditions more representative of long-term equilibrium. Here, we have used bulk geochemical and microbial community analysis of soils, coupled with X-ray absorption spectroscopy and mu-focus X-ray fluorescence mapping, to gain a mechanistic understanding of the fate of U transported into an organic-rich soil from a pitchblende vein at the UK Needle's Eye Natural Analogue site. U is highly enriched in the Needle's Eye soils (similar to 1600 mg kg(-1)). We show that this enrichment is largely controlled by U(VI) complexation with soil organic matter and not U(VI) bioreduction. Instead, organic-associated U(VI) seems to remain stable under microbially-mediated Fe(III)-reducing conditions. U(IV) (as non-crystalline U(IV)) was only observed at greater depths at the site (>25 cm); the soil here was comparatively mineral-rich, organic-poor, and sulfate-reducing/methanogenic. Furthermore, nanocrystalline UO2, an alternative product of U(VI) reduction in soils, was not observed at the site, and U did not appear to be associated with Fe-bearing minerals. Organicrich soils appear to have the potential to impede U groundwater transport, irrespective of ambient redox conditions. (C) 2020 The Authors. Published by Elsevier Ltd.

Originalspråkengelska
Artikelnummer126859
TidskriftChemosphere
Volym254
Antal sidor9
ISSN0045-6535
DOI
StatusPublicerad - sep 2020
MoE-publikationstypA1 Tidskriftsartikel-refererad

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