Sequential scavenging and measurement of seawater radiocesium concentrations and plutonium isotopic ratios offshore Fukushima

Abstract

The scientific interest in radiocesium and plutonium found in the oceans and seas has increased enormously in the past years as a consequence of the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident and is expected to be ongoing due to many unresolved questions. Hence, continuous development of new and verification of old analytical methods should be at the top of the list of the community, working on the topic. In this study, we processed and analyzed several seawater samples, collected in different time frames (2011-2015) from the North Pacific Ocean offshore Fukushima, to determine their radiocesium activities, ¹³⁴Cs/¹³⁷Cs activity ratios and ²⁴⁰Pu/²³⁹Pu isotopic ratios using the sequential scavenging method, gamma spectrometry and accelerator mass spectrometry (AMS). The observed radiocesium levels in seawater (0.07-0.042 Bq L^-1) clearly indicated that the investigated region remained impacted by releases from the damaged power plant even after four years after the accident. Regarding plutonium, its successful separation from large volume seawater samples was confirmed by detection of ²⁴⁰Pu by AMS. However, several problems emerged during the analyzes, which we tried to address with the use of additional methods (e.g., measurements of uranium by ICPMS). The efficiencies of the applied methods and other issues are also discussed.

Keywords: AMS; Fukushima; Gamma spectrometry; Plutonium; Radiocesium; seawater.