Synchrotron-Based X-ray Fluorescence Imaging Elucidates Uranium Toxicokinetics in Daphnia magna.

A combination of synchrotron-based elemental analysis and acute toxicity tests was used to investigate the biodistribution and adverse effects in Daphnia magna exposed to uranium nanoparticle (UNP, 3-5 nm) suspensions or to uranium reference (Uref) solutions. Speciation analysis revealed similar size distributions between exposures, and toxicity tests showed comparable acute effects (UNP LC50: 402 µg L-1 [336-484], Uref LC50: 268 µg L-1 [229-315]). However, the uranium body burden was 3- to 5-fold greater in UNP-exposed daphnids, and analysis of survival as a function of body burden revealed a ∼5-fold higher specific toxicity from the Uref exposure. High-resolution X-ray fluorescence elemental maps of intact, whole daphnids from sublethal, acute exposures of both treatments revealed high uranium accumulation onto the gills (epipodites) as well as within the hepatic ceca and the intestinal lumen. Uranium uptake into the hemolymph circulatory system was inferred from signals observed in organs such as the heart and the maxillary gland. The substantial uptake in the maxillary gland and the associated nephridium suggests that these organs play a role in uranium removal from the hemolymph and subsequent excretion. Uranium was also observed associated with the embryos and the remnants of the chorion, suggesting uptake in the offspring. The identification of target organs and tissues is of major importance to the understanding of uranium and UNP toxicity and exposure characterization that should ultimately contribute to reducing uncertainties in related environmental impact and risk assessments.

Synchrotron XRF and Histological Analyses Identify Damage to Digestive Tract of Uranium NP-Exposed Daphnia magna.

Micro- and nanoscopic X-ray techniques were used to investigate the relationship between uranium (U) tissue distributions and adverse effects to the digestive tract of aquatic model organism Daphnia magna following uranium nanoparticle (UNP) exposure. X-ray absorption computed tomography measurements of intact daphnids exposed to sublethal concentrations of UNPs or a U reference solution (URef) showed adverse morphological changes to the midgut and the hepatic ceca. Histological analyses of exposed organisms revealed a high proportion of abnormal and irregularly shaped intestinal epithelial cells. Disruption of the hepatic ceca and midgut epithelial tissues implied digestive functions and intestinal barriers were compromised. Synchrotron-based micro X-ray fluorescence (XRF) elemental mapping identified U co-localized with morphological changes, with substantial accumulation of U in the lumen as well as in the epithelial tissues. Utilizing high-resolution nano-XRF, 400-1000 nm sized U particulates could be identified throughout the midgut and within hepatic ceca cells, coinciding with tissue damages. The results highlight disruption of intestinal function as an important mode of action of acute U toxicity in D. magna and that midgut epithelial cells as well as the hepatic ceca are key target organs.

Characterization of radioactive particles from the Dounreay nuclear reprocessing facility.

Radioactive particles originating from nuclear fuel reprocessing at the United Kingdom Atomic Energy Authority's Dounreay Facility were inadvertently released to the environment in the late 1950s to 1970s and have subsequently been found on site grounds and local beaches. Previous assessments of risk associated with encountering a particle have been based on conservative assumptions related to particle composition and speciation. To reduce uncertainties associated with environmental impact assessments from Dounreay particles, further characterization is relevant. Results of particles available for this study showed variation between Dounreay Fast Reactor (DFR) and Materials Test Reactor (MTR) particles, reflecting differences in fuel design, release scenarios, and subsequent environmental influence. Analyses of DFR particles showed they are small (100-300 µm) and contain spatially correlated U and Nb. Molybdenum, part of the DFR fuel, was identified at atomic concentrations below 1%. Based on SR-based micrometer-scale X-ray Absorption Near Edge Structure spectroscopy (µ-XANES), U may be present as U(IV), and, based on a measured Nb/U atom ratio of ~2, stoichiometric considerations are commensurable with the presence of UNb2O7. The MTR particles were larger (740-2000 µm) and contained U and Al inhomogeneously distributed. Neodymium (Nd) was identified in atomic concentrations of around 1-2%, suggesting it was part of the fuel design. The presence of U(IV) in MTR particles, as indicated by µ-XANES analysis, may be related to oxidation of particle surfaces, as could be expected due to corrosion of UAlx fuel particles in air. High 235U/238U atom ratios in individual DFR (3.2 ± 0.8) and MTR (2.6 ± 0.4) particles reflected the presence of highly enriched uranium. The DFR particles featured lower 137Cs activity levels (2.00-9.58 kBq/particle) than the MTR (43.2-641 kBq 137Cs/particle) particles. The activities of the dose contributing radionuclides 90Sr/90Y were proportional to 137Cs (90Sr/137Cs activity ratio ≈ 0.8) and particle activities were roughly proportional to the size. Based on direct beta measurements, gamma spectrometry, and the VARSKIN6 model, contact dose rates were calculated to be approximately 74 mGy/h for the highest activity MTR particle, in agreement with previously published estimates.

Behavior of 137Cs in ponds in the vicinity of the Fukushima Dai-ichi nuclear power plant.

137Cs activity concentration in the water of four ponds, Suzuuchi (SU), Funasawa (FS), Inkyozaka (IZ), and Kashiramori (KM), that are within 10 km of the Fukushima Dai-ichi nuclear power plant were observed from April 2015 to August 2016. 137Cs inventories in soils surrounding SU, FS, IZ, and KM were 6.4, 2.9, 2.1, and 0.9 MBq m-2, respectively. 137Cs inventories in the bottom sediments of SU, FS, IZ, and KM were 13, 8.9, 1.6, and 1.1 MBq m-2, respectively. Higher 137Cs inventories in bottom sediment than those of soil in SU and FS suggest that 137Cs was delivered to and accumulated in these ponds. Mean total 137Cs activity concentrations in SU, FS, IZ, and KM were 41, 13, 9.5, and 1.4 Bq L-1, respectively. Particulate 137Cs concentration accounted for 71-90% of total 137Cs in the water samples, on average. The mean distribution coefficient, Kd, in SU, FS, IZ, and KM was 1.3 × 105, 2.1 × 105, 1.7 × 105, and 6.2 × 105 L kg-1, respectively. These Kd values were higher than the Kd values observed in the Chernobyl area by 1-2 orders of magnitude. Although no significant decreasing trends were found, dissolved 137Cs activity concentration tended to be low during winter in all four ponds. Dissolved 137Cs activity concentrations were proportional to K+ and DOC concentrations in all the ponds. The results from principal component analysis performed for 137Cs activity concentration and water chemistry data sets suggested that there were different mechanisms behind variability of dissolved 137Cs activity concentrations for each pond. Continuous monitoring is required to reveal temporal trends in 137Cs activity concentrations of these waters and controlling factors of such in closed water systems in Fukushima.