Natural and anthropogenic radionuclide distributions in the northwest Atlantic Ocean

We have used in-situ pumps which filter large volumes of sea water through a 1 μm cartridge prefilter and two MnO₂-coated cartridges to obtain information on dissolved and particulate radionuclide distributions in the oceans. Two sites in the northwest Atlantic show subsurface maxima of the fallout radionuclides¹³⁷Cs,^239,240Pu and²⁴¹Am. Although the processes of scavenging onto sinking particles and release at depth may contribute to the tracer distributions, comparison of predicted and measured water column inventories suggests that at least 35–50% of the Pu and²⁴¹Am are supplied to the deep water by advection.The depth distributions of the naturally occurring radionuclides²³²Th,²²⁸Th and²³⁰Th reflect their sources to the oceans.²³²Th shows high dissolved concentrations in surface waters, presumably as a result of atmospheric or riverine supply. Activities of²³²Th decrease with depth to values 0.01 dpm/1000 l.²²⁸Th shows high activities in near surface and near bottom water, due to the distribution of its parent,²²⁸Ra. Dissolved²³⁰Th, produced throughout the water column from²³⁴U decay, increases with depth to 3000 m. Values in the deep water (> 3000 m) are nearly constant ( 0.6–0.7 dpm/1000 l), and the distribution of this tracer (and perhaps other long-lived particle-reactive tracers as well) may be affected by the advection inferred from Pu and²⁴¹Am data.The ratio of particulate to dissolved activity for both²³⁰Th and²²⁸Th is 0.15–0.20. This similarity precludes the calculation of sorption rate constants using a simple model of reversible sorption equilibrium. Moreover, in mid-depths²²⁸Th tends to have a higher particulate/dissolved ratio than²³⁰Th, suggesting uptake and release of²³⁰Th and²²⁸Th by different processes. This could occur if²²⁸Th, produced in surface water, were incorporated into biogenic particles formed there and released as those particles dissolved or decomposed during sinking.²³⁰Th, produced throughout the water column, may more closely approach a sorption equilibrium at all depths.²³⁰Th,²⁴¹Am and^239,240Pu are partitioned onto particles in the sequence Th > Am > Pu with 15% of the²³⁰Th on particles compared with 7% for Am and 1% for Pu. Distribution coefficients (K_d) are 1.3–1.6 × 10⁷ for Th, 5–6 × 10⁶ for Am and 7–10 × 10⁵ for Pu. The lower reactivity for Pu is consistent with analyses of Pu oxidation states which show 85% oxidized (V + VI) Pu. However, theK_d value for Pu may be an upper limit because Pu, like²²⁸Th, may be incorporated into particles in surface waters and released at depth only by destruction of the carrier phase.