Anthropogenic ²³⁶U and ²³³U in the Baltic Sea: Distributions, source terms, and budgets

The Baltic Sea receives substantial amounts of hazardous substances and nutrients, which accumulate for decades and persistently impair the Baltic ecosystems. With long half-lives and high solubility, anthropogenic uranium isotopes (²³⁶U and ²³³U) are ideal tracers to depict the ocean dynamics in the Baltic Sea and the associated impacts on the fates of contaminants. However, their applications in the Baltic Sea are hampered by the inadequate source-term information. This study reports the first three-dimensional distributions of ²³⁶U and ²³³U in the Baltic Sea (2018–2019) and the first long-term hindcast simulation for reprocessing-derived ²³⁶U dispersion in the North-Baltic Sea (1971–2018). Using ²³³U/²³⁶U fingerprints, we distinguish ²³⁶U from the nuclear weapon testing and civil nuclear industries, which have comparable contributions (142 ± 13 and 174 ± 40 g) to the ²³⁶U inventory in modern Baltic seawater. Budget calculations for ²³⁶U inputs since the 1950s indicate that, the major ²³⁶U sources in the Baltic Sea are the atmospheric fallouts (∼1.35 kg) and discharges from nuclear reprocessing plants (> 211 g), and there is a continuous sink of ²³⁶U to the anoxic sediments (589 ± 43 g). Our findings also indicate that the limited water renewal endows the Baltic Sea a strong "memory effect" retaining aged ²³⁶U signals, and the previously unknown ²³⁶U in the Baltic Sea is likely attributed to the retention of the mid-1990s' discharges from the nuclear reprocessing plants. Our preliminary results demonstrate the power of ²³⁶U-¹²⁹I dual-tracer in investigating water-mass mixing and estimating water age in the Baltic Sea, and this work provides fundamental knowledge for future ²³⁶U tracer studies in the Baltic Sea.