Physico-Chemical Heterogeneity of Organic-Rich Sediments in the Rifle Aquifer, CO: Impact on Uranium Biogeochemistry

Janot, Noémie; Lezama Pacheco, Juan S.; Pham, Don Q.; O’Brien, Timothy M.; Hausladen, Debra; Noël, Vincent; Lallier, Florent; Maher, Kate; Fendorf, Scott; Williams, Kenneth H.; Long, Philip E.; Bargar, John R.

doi:10.1021/acs.est.5b03208

Physico-Chemical Heterogeneity of Organic-Rich Sediments in the Rifle Aquifer, CO: Impact on Uranium Biogeochemistry

Journal Article · Wed Dec 09 23:00:00 EST 2015 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.5b03208· OSTI ID:1471003

Janot, Noémie ^[1]; Lezama Pacheco, Juan S. ^[2]; Pham, Don Q. ^[1]; O’Brien, Timothy M. ^[1]; Hausladen, Debra ^[3]; Noël, Vincent ^[1]; Lallier, Florent ^[4]; Maher, Kate ^[5]; Fendorf, Scott ^[3]; Williams, Kenneth H. ^[6]; Long, Philip E. ^[6]; Bargar, John R. ^[1]

SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Stanford Univ., CA (United States). Dept. of Environmental Earth System Science
Stanford Univ., CA (United States). Dept. of Environmental Earth System Science
Univ. de Lorraine, Vandœuvre-lès-Nancy (France)
Stanford Univ., CA (United States). Dept. of Geological Sciences
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Earth Sciences Division

The Rifle alluvial aquifer along the Colorado River in west central Colorado contains fine-grained, diffusion-limited sediment lenses that are substantially enriched in organic carbon and sulfides, as well as uranium, from previous milling operations. These naturally reduced zones (NRZs) coincide spatially with a persistent uranium groundwater plume. There is concern that uranium release from NRZs is contributing to plume persistence or will do so in the future. To better define the physical extent, heterogeneity and biogeochemistry of these NRZs, we investigated sediment cores from five neighboring wells. The main NRZ body exhibited uranium concentrations up to 100 mg/kg U as U(IV) and contains ca. 286 g of U in total. Uranium accumulated only in areas where organic carbon and reduced sulfur (as iron sulfides) were present, emphasizing the importance of sulfate-reducing conditions to uranium retention and the essential role of organic matter. NRZs further exhibited centimeter-scale variations in both redox status and particle size. Mackinawite, greigite, pyrite and sulfate coexist in the sediments, indicating that dynamic redox cycling occurs within NRZs and that their internal portions can be seasonally oxidized. In conclusion, we show that oxidative U(VI) release to the aquifer has the potential to sustain a groundwater contaminant plume for centuries. NRZs, known to exist in other uranium-contaminated aquifers, may be regionally important to uranium persistence.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

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

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1471003

Alternate ID(s):: OSTI ID: 1256968

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 1 Vol. 50; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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