Plutonium mobilization from contaminated estuarine sediments, Esk Estuary (UK).

Since 1952, liquid radioactive effluent containing238-242Pu, 241Am, 237Np, 137Cs, and 99Tc has been released with authorization from the Sellafield nuclear complex (UK) into the Irish Sea. This represents the largest source of plutonium (Pu) discharged in all western Europe, with 276 kg having been released. In the Eastern Irish Sea, the majority of the transuranic activity has settled into an area of sediments (Mudpatch) located off the Cumbrian coast. Radionuclides from the Mudpatch have been re-dispersed via particulate transport in fine-grained estuarine and intertidal sediments to the North-East Irish Sea, including the intertidal saltmarsh located at the mouth of the Esk Estuary. Saltmarshes are highly dynamic systems which are vulnerable to external agents (sea level change, erosion, sediment supply, and freshwater inputs), and their stability remains uncertain under current sea level rise projections and possible increases in storm activity. In this work, we examined factors affecting Pu mobility in contaminated sediments collected from the Esk Estuary by conducting leaching experiments under both anoxic and oxic conditions. Leaching experiments were conducted over a 9-month period and were periodically sampled to determine solution phase Pu via multicollector-inductively coupled plasma-mass spectrometry (MC-ICP-MS), and to measure redox indicators (Eh, pH and extractable Fe(II)). Microbial community composition was also characterized in the sediments, and at the beginning and end of the anoxic/oxic experiments. Results show that: 1) Pu leaching is about three times greater in solutions leached under anoxic conditions compared to oxic conditions, 2) the sediment slurry microbial communities shift as conditions change from anoxic to oxic, 3) Pu leaching is enhanced in the shallow sediments (0-10 cm depth), and 4) the magnitude of Pu leached from sediments is not correlated with total Pu, indicating that the biogeochemistry of sediment-associated Pu is spatially heterogeneous. These findings provide constraints on the stability of redox sensitive Pu in biogeochemically dynamic/transient environments on a timescale of months and suggests that anoxic conditions can enhance Pu mobility in estuarine systems.

U-Pb constraints on pulsed eruption of the Deccan Traps across the end-Cretaceous mass extinction.

Temporal correlation between some continental flood basalt eruptions and mass extinctions has been proposed to indicate causality, with eruptive volatile release driving environmental degradation and extinction. We tested this model for the Deccan Traps flood basalt province, which, along with the Chicxulub bolide impact, is implicated in the Cretaceous-Paleogene (K-Pg) extinction approximately 66 million years ago. We estimated Deccan eruption rates with uranium-lead (U-Pb) zircon geochronology and resolved four high-volume eruptive periods. According to this model, maximum eruption rates occurred before and after the K-Pg extinction, with one such pulse initiating tens of thousands of years prior to both the bolide impact and extinction. These findings support extinction models that incorporate both catastrophic events as drivers of environmental deterioration associated with the K-Pg extinction and its aftermath.

Volcanic-plutonic parity and the differentiation of the continental crust.

The continental crust is central to the biological and geological history of Earth. However, crustal heterogeneity has prevented a thorough geochemical comparison of its primary igneous building blocks-volcanic and plutonic rocks-and the processes by which they differentiate to felsic compositions. Our analysis of a comprehensive global data set of volcanic and plutonic whole-rock geochemistry shows that differentiation trends from primitive basaltic to felsic compositions for volcanic versus plutonic samples are generally indistinguishable in subduction-zone settings, but are divergent in continental rifts. Offsets in major- and trace-element differentiation patterns in rift settings suggest higher water content in plutonic magmas and reduced eruptibility of hydrous silicate magmas relative to dry rift volcanics. In both tectonic settings, our results indicate that fractional crystallization, rather than crustal melting, is predominantly responsible for the production of intermediate and felsic magmas, emphasizing the role of mafic cumulates as a residue of crustal differentiation.

Earth history. U-Pb geochronology of the Deccan Traps and relation to the end-Cretaceous mass extinction.

The Chicxulub asteroid impact (Mexico) and the eruption of the massive Deccan volcanic province (India) are two proposed causes of the end-Cretaceous mass extinction, which includes the demise of nonavian dinosaurs. Despite widespread acceptance of the impact hypothesis, the lack of a high-resolution eruption timeline for the Deccan basalts has prevented full assessment of their relationship to the mass extinction. Here we apply uranium-lead (U-Pb) zircon geochronology to Deccan rocks and show that the main phase of eruptions initiated ~250,000 years before the Cretaceous-Paleogene boundary and that >1.1 million cubic kilometers of basalt erupted in ~750,000 years. Our results are consistent with the hypothesis that the Deccan Traps contributed to the latest Cretaceous environmental change and biologic turnover that culminated in the marine and terrestrial mass extinctions.