Plutonium Isotopes (^239–241Pu) Dissolved in Pacific Ocean Waters Detected by Accelerator Mass Spectrometry: No Effects of the Fukushima Accident Observed

Abstract

The concentration of plutonium (Pu) and the isotopic ratios of ²⁴⁰Pu to ²³⁹Pu and ²⁴¹Pu to ²³⁹Pu were determined by accelerator mass spectrometry (AMS) in Pacific Ocean water samples (20 L each) collected in late 2012. The isotopic Pu ratios are important indicators of different contamination sources and were used to identify a possible release of Pu into the ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. In particular, ²⁴¹Pu is a well-suited indicator for a recent entry of Pu because ²⁴¹Pu from fallout of nuclear weapon testings has already significantly decayed. A total of 10 ocean water samples were prepared at the Radiochemie München of the TUM and analyzed at the Vienna Environmental Research Laboratory (VERA). Several samples showed a slightly elevated ²⁴⁰Pu/²³⁹Pu ratio of up to 0.22 ± 0.02 compared to global fallout (²⁴⁰Pu/²³⁹Pu = 0.180 ± 0.007), whereas all measured ²⁴¹Pu-to-²³⁹Pu ratios were consistent with nuclear weapon fallout (²⁴¹Pu/²³⁹Pu < 2.4 × 10^-3), which means that no impact from the Fukushima accident was detected. From the average ²⁴¹Pu-to-²³⁹Pu ratio of 8_-2⁺³ ×10^-4 at a sampling station located at a distance of 39.6 km to FDNPP, the 1-σ upper limit for the FDNPP contribution to the ²³⁹Pu inventory in the water column was estimated to be 0.2%. Pu, with the signature of weapon-grade Pu was found in a single sample collected around 770 km off the west coast of the United States.