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中国九龙江口表层水体中不同粒径分级的钍同位素(228Th、230Th、232Th)

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

作者信息

Zhang Lei, Chen Min, Yang Weifeng, Xing Na, Li Yanping, Qiu Yusheng, Huang Yipu

机构信息

Department of Oceanography, Xiamen University, Xiamen 361005, China.

出版信息

J Environ Radioact. 2005;78(2):199-216. doi: 10.1016/j.jenvrad.2004.05.004.

Abstract

Thorium isotopes (228Th, 230Th, 232Th and 234Th) 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 228Th, 230Th and 232Th in different size fractions, namely, the >53 microm, 10-53 microm, 2-10 microm, 0.4-2 microm, 10 kDa-0.4 microm and the <10 kDa fractions. Our results indicated that the activity concentrations of 228Th, 230Th and 232Th 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 particulate 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 microm fraction had the least share (0-1%), while the 10-53 microm fraction had the largest share of Th isotopes. The average value of the 230Th/232Th activity ratio (230Th/232Th)(A.R.) increased from 0.8 in the >53 microm fraction to 3.7 in the 10 kDa-0.4 microm fraction, indicating that the radiogenic Th isotopes are preferentially scavenged by the small size particles. (230Th/232Th)(A.R.) in the <10 kDa and 10 kDa-0.4 microm fractions were similar, however, suggesting a similar chemical composition and/or equilibrium partitioning between the low 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 228Th had the highest concentration in the mid-salinity region, showing a non-conservative behavior with additional input. In contrast, dissolved 232Th showed a concave profile, indicating a net removal of 232Th 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.

摘要

钍同位素(228Th、230Th、232Th和234Th)是研究海洋环境中颗粒动力学和微量元素清除的有用示踪剂。在本研究中,沿着中国九龙江河口的盐度梯度采集了表层水,以测定不同粒径组分(即>53微米、10 - 53微米、2 - 10微米、0.4 - 2微米、10 kDa - 0.4微米和<10 kDa组分)中228Th、230Th和232Th的活度浓度。我们的结果表明,九龙江河口水中228Th、230Th和232Th的活度浓度显著高于先前报道的大多数沿海和海洋海水中的值,这表明九龙江流域对陆源铀和钍的贡献更高。当以颗粒质量浓度进行归一化时,三种钍同位素的活度浓度随颗粒粒径增大而降低,这表明颗粒表面积在控制水柱中钍的清除方面起着重要作用。三种钍同位素的分配表现出一个共同特征,即>53微米的组分所占份额最少(0 - 1%),而10 - 53微米的组分对钍同位素的份额最大。230Th/232Th活度比(230Th/232Th)(A.R.)的平均值从>53微米组分中的0.8增加到10 kDa - 0.4微米组分中的3.7,这表明放射性钍同位素优先被小粒径颗粒清除。然而,<10 kDa和10 kDa - 0.4微米组分中的(230Th/232Th)(A.R.)相似,这表明低分子量和胶体态钍之间具有相似的化学组成和/或平衡分配。非常有趣的是,三种钍同位素的地球化学行为彼此不同。溶解态228Th在中等盐度区域浓度最高,表现出非保守行为且有额外输入。相反地,溶解态232Th呈现出凹形曲线,表明在淡水与海水混合过程中232Th有净去除。<10 kDa组分中钍同位素的行为与溶解相中的行为一致。三种钍同位素地球化学行为的差异归因于它们在河口的不同来源。

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