Distribution of plutonium and americium in the marginal seas of the northwest Pacific Ocean

Abstract

Plutonium isotopes and Am-241 were studied in seawater and sediment from the East China Sea, the Yellow Sea, the East Sea/Sea of Japan, the Sea of Okhotsk, and the northwest Pacific Ocean, collected between 1993 and 1996 with the aim to contribute to better understanding the behaviour of plutonium and americium in the marine environment. Pu-239,Pu-240, concentrations in surface water varied from 2.3 to 13 muBq l(-1) in the East China Sea and from 3.5 to 9.4 muBq l(-1) in the East Sea. The 211,211PU vertical profiles in water showed a broad subsurface maximum between 500 and 1000 m with a range of 30-40 muBq l(-1), and gradually decreased from 1000 m depth down to the seafloor. 24 Am concentrations in surface water showed values from 1.1 to 2.2 mubetal(-1) l(-1) in the East Sea, from 1.0 to 3.1 muBq l(-1) in the Sea of Okhotsk, and from 0.68 to 12.0 muBq l(-1) in the northwest Pacific Ocean. The activity ratios of Am-24 /239,240 Pu in seawater showed values similar to the global fallout ratio, which suggests that the source of these radionuclides in the northwest Pacific Ocean is global fallout. However, the (241) Am/(239,40) Pu activity ratios in sediment were found to be much higher (1.0-1.9) than the global fallout ratio (0.37), confirming that Am-241 is scavenged from the water column more rapidly than (239,240) Pu. The 239,240Pu inventories in the water column of the East Sea were from 0.98 to 93 Bq m(-2) depending on water depth and sedimentation rates. The Am-241 inventory in the water column east of Kamchatka was 6.3 + 1.0 Bq m(-2) and the sediment inventory in the Sea of Okhotsk was 16+/-2 Bq M-2. Pu-219,Pu-240 concentrations in sinking particles in the southwest Japan Basin were from 3.7 to 5.2 Bq kg(-1) (dry weight) with fluxes of 0.194.50 mBq m(-2) d(-1) and at the Ulleung Basin from 2.4 to 3.7 Bq kg(-1) (dry weight) with fluxes of 0.771.10 mBq m(-2) d(-1). The mean residence time of 239,240Pu in the water column of the East Sea derived from sediment trap data was 140+/-20 years, 2-3 times less than in the Atlantic and Pacific oceans. (C) 2003 Elsevier Ltd. All rights reserved.