Redox Controls over the Stability of U(IV) in Floodplains of the Upper Colorado River Basin

Noel, Vincent; Boye, Kristin; Lezama Pacheco, Juan S.; Bone, Sharon E.; Janot, Noemie; Cardarelli, Emily; Williams, Kenneth H.; Bargar, John R.

doi:10.1021/acs.est.7b02203

Redox Controls over the Stability of U(IV) in Floodplains of the Upper Colorado River Basin

Journal Article · Tue Sep 05 00:00:00 EDT 2017 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.7b02203· OSTI ID:1457054

^[1]; Boye, Kristin ^[2]; Lezama Pacheco, Juan S. ^[2]; Bone, Sharon E. ^[1]; Janot, Noemie ^[1]; Cardarelli, Emily ^[3]; Williams, Kenneth H. ^[4]; ^[1]

SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
Stanford Univ., Stanford, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Here, aquifers in the Upper Colorado River Basin (UCRB) exhibit persistent uranium (U) groundwater contamination plumes originating from former ore processing operations. Previous observations at Rifle, Colorado, have shown that fine grained, sulfidic, organic-enriched sediments accumulate U in its reduced form, U(IV), which is less mobile than oxidized U(VI). These reduced sediment bodies can subsequently act as secondary sources, releasing U back to the aquifer. There is a need to understand if U(IV) accumulation in reduced sediments is a common process at contaminated sites basin-wide, to constrain accumulated U(IV) speciation, and to define the biogeochemical factors controlling its reactivity. We have investigated U(IV) accumulation in organic-enriched reduced sediments at three UCRB floodplains. Noncrystalline U(IV) is the dominant form of accumulated U, but crystalline U(IV) comprises up to ca. 30% of total U at some locations. Differing susceptibilities of these species to oxidative remobilization can explain this variability. Particle size, organic carbon content, and pore saturation, control the exposure of U(IV) to oxidants, moderating its oxidative release. Further, our data suggest that U(IV) can be mobilized under deeply reducing conditions, which may contribute to maintenance and seasonal variability of U in groundwater plumes in the UCRB.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515

OSTI ID:: 1457054

Alternate ID(s):: OSTI ID: 1476551

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 19 Vol. 51; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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