Sources and scavenging of plutonium in the East China Sea

The ²⁴⁰Pu/²³⁹Pu atom ratio and ^239+240Pu activity of seawater in the East China Sea (ECS) was measured in order to examine the Pu sources and elaborate Pu scavenging process. High ²⁴⁰Pu/²³⁹Pu atom ratios (0.187-0.243, average = 0.221 ± 0.017) in the surface water and water column were observed during 2011, implying of non-global fallout Pu sources. The distribution of ²⁴⁰Pu/²³⁹Pu atom ratio in the ECS was in agreement with the introduction pathway of the Kuroshio, showing a decreasing trend away from the outer shelf. An even higher ²⁴⁰Pu/²³⁹Pu atom ratios (0.243-0.263, average = 0.253 ± 0.007) were observed in the Kuroshio, indicating the non-global fallout Pu signal from the Pacific Proving Grounds (PPG). Using a two end-member mixing model, the Pu source from the PPG contribution was calculated to be 36 ± 9% in the ECS seawater. The ^239+240Pu activities of surface seawater were in the range of 2.00-2.95 mBq m^-3 in the ECS. The spatial distribution of ^239+240Pu activity in the surface seawater showed an increasing trend from the outer shelf to the nearshore. Moreover, ^239+240Pu inventory of water column at the station DH23 in the ECS was calculated to be ~0.29 Bq m^-2, which was 1-3 orders of magnitude lower than the estimates of sediment cores in the ECS shelf (9-407 Bq m^-2). Such differences were determined by the high degree Pu scavenging efficiency in the ECS and high Pu input carried by terrestrial sediments from the Yangtze River. Finally, both ²⁴⁰Pu/²³⁹Pu atom ratios and ^239+240Pu activities were identical before and after the Fukushima nuclear accident (FNA), suggesting that the impact of the FNA on the ECS was negligible.