Uranium diagenesis in sediments underlying bottom waters with high oxygen content

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Morford, Jennifer L.
Martin, William R.
Carney, Caitlin M.
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We measured U in sediments (both pore waters and solid phase) from three locations on the middle Atlantic Bight (MAB) from the eastern margin of the United States: a northern location on the continental shelf off Massachusetts (OC426, 75 m water depth), and two southern locations off North Carolina (EN433-1, 647 m water depth and EN433-2, 2648 m water depth). These sediments underlie high oxygen bottom waters (250-270 μM), but become reducing below the sediment-water interface due to the relatively high organic carbon oxidation rates in sediments (EN433-1: 212 μmol C/cm2/y; OC426: 120±10 μmol C/cm2/y; EN433-2: 33 μmol C/cm2/y). Pore water oxygen goes to zero by 1.4-1.5 cm at EN433-1 and OC426 and slightly deeper oxygen penetration depths were measured at EN433-2 (~4 cm). All of the pore water profiles show removal of U from pore waters. Calculated pore water fluxes are greatest at EN433-1 (0.66±0.08 nmol/cm2/y) and less at EN433-2 and OC426 (0.24±0.05 and 0.13±0.05 nmol/cm2/y, respectively). Solid phase profiles show authigenic U enrichment in sediments from all three locations. The average authigenic U concentrations are greater at EN433-1 and OC426 (5.8±0.7 nmol/g and 5.4±0.2 nmol/g, respectively) relative to EN433-2 (4.1±0.8 nmol/g). This progression is consistent with their relative ordering of ‘reduction intensity’, with greatest reducing conditions in sediments from EN433-1, less at OC426 and least at EN433-2. The authigenic U accumulation rate is largest at EN433-1 (0.47±0.05 nmol/cm2/y), but the average among the three sites on the MAB is ~0.2 nmol/cm2/y. Pore water profiles suggest diffusive fluxes across the sediment-water interface that are 1.4-1.7 times greater than authigenic accumulation rates at EN433-1 and EN433-2. These differences are consistent with oxidation and loss of U from the solid phase via irrigation and/or bioturbation, which may compromise the sequestration of U in continental margin sediments that underlie bottom waters with high oxygen concentrations. Previous literature compilations that include data exclusively from locations where [O2]bw < 150 μM suggest compelling correlations between authigenic U accumulation and organic carbon flux to sediments or organic carbon burial rate. Sediments that underlie waters with high [O2]bw have lower authigenic U accumulation rates than would be predicted from relationships developed from results that include locations where [O2]bw < 150 μM.
Author Posting. © The Author(s), 2009. This is the author's version of the work. It is posted here by permission of Elsevier B.V. for personal use, not for redistribution. The definitive version was published in Geochimica et Cosmochimica Acta 73 (2009): 2920-2937, doi:10.1016/j.gca.2009.02.014.
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