Size-fractionated thorium isotopes (~(228)Th, ~(230)Th, ~(232)Th) in surface waters in the Jiulong River estuary, China

摘要

Thorium isotopes (~(228)Th, ~(230)Th, ~(232)Th and ~(234)Th) are useful tracers for studying particle dynamics and trace element scavenging in marine environments. In this study, surface waters were collected along a salinity gradient from the Jiulong River estuary, China, for determination of activity concentrations of ~(228)Th, ~(230)Th and ~(232)Th in different size fractions, namely, the >53 μm, 10-53 μm, 2-10 μm, 0.4-2 μm, 10 kDa-0.4 μm and the < 10 kDa fractions. Our results indicated that the activity concentrations of ~(228)Th, ~(230)Th and ~(232)Th in the Jiulong River estuarine waters were significantly higher than most of the previously reported values in coastal and oceanic seawaters, suggesting a higher lithogenic U and Th contribution from the Jiulong River Basin. When normalized to the paniculate mass concentration, the activity concentrations of the three thorium isotopes decreased with increasing particle size, demonstrating the important role of surface areas of particles in controlling the scavenging of thorium from the water column. The partitioning of three thorium isotopes showed a common characteristic, i.e., the >53 μm fraction had the least share (0-1%), while the 10-53 μm fraction had the largest share of Th isotopes. The average value of the ~(230)Th/~(232)Th activity ratio (~(230)Th/~(232)Th)_(A.R.). increased from 0.8 in the > 53 μm fraction to 3.7 in the 10 kDa-0.4 μm fraction, indicating that the radiogenic Th isotopes are preferentially scavenged by the small size particles. (~(230)Th/~(232)Th)_(A.R). in the < 10 kDa and 10 kDa-0.4 μm fractions were similar, however, suggesting a similar chemical composition and/or equilibrium partitioning between the !ow molecular weight and colloidal Th. It was very interesting to note that the geochemical behaviors of the three Th isotopes were different from each other. Dissolved ~(228)Th had the highest concentration in the mid-salinity region, showing a non-conservative behavior with additional input. In contrast, dissolved ~(232)Th showed a concave profile, indicating a net removal of ~(232)Th during the mixing of fresh water with seawater. The behavior of Th isotopes in the < 10 kDa fraction followed those in the dissolved phases. The difference in geochemical behaviors among three Th isotopes was ascribed to their different sources in the estuary.