Pu Isotopic Composition Indicates Its Sources and Environmental Changes in the Vicinity of Daya Bay Nuclear Power Plant

IF 2.9 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

ACS Earth and Space Chemistry Pub Date : 2025-01-10 DOI:10.1021/acsearthspacechem.4c0029010.1021/acsearthspacechem.4c00290

Jisheng Chen, Panpan Yang, Wenting Bu*, Ke Xiong, Cui Wang, Xiuli Yan, Yong Liu, Peng Wu and Junwen Wu*,

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Abstract

The plutonium (Pu) isotopic compositions of surface sediments and two sediment cores from Daya Bay were measured by ICP–MS for the sake of investigating the sources of Pu and their historical evolution. The surface ²⁴⁰Pu/²³⁹Pu atomic ratios in Daya Bay are in the range of 0.247–0.287 (average = 0.264 ± 0.011, n = 14), which are higher than the characteristic value of global fallout (∼0.178) and indicate the input from non-global fallout. Correspondingly, the ^239+240Pu activities were in the range of 0.029–0.386 Bq kg^–1 (average = 0.197 ± 0.091 Bq kg^–1, n = 14), and their spatial distribution shows relatively high Pu activity at the mouth and western part of Daya Bay, which is mainly attributed to finer particle sizes. The high ²⁴⁰Pu/²³⁹Pu atomic ratios were confirmed to be from the contribution to Pacific Proving Grounds (65% ± 7%) transported via the Kuroshio current. There was no additional Pu input released from the normal operation of Daya Bay nuclear power plants. Additionally, the Pu chronology of the sediment cores showed that changes in the sedimentary environment impact the Pu isotopic content. The Advection-Diffusion Equation model was used to further evaluate and predict the vertical migration of Pu isotopes in Daya Bay, suggesting that the diffusion of Pu over time may impact its usefulness as a time marker. Finally, we provide a baseline value of Pu isotopes in Daya Bay for environmental risk assessments in the future.

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为研究大亚湾钚的来源及其历史演变，采用 ICP-MS 测量了大亚湾表层沉积物和两个沉积岩芯的钚（Pu）同位素组成。大亚湾地表240Pu/239Pu原子比值在0.247-0.287之间（平均值=0.264±0.011，n=14），高于全球沉降物的特征值（∼0.178），表明非全球沉降物的输入。相应地，239+240Pu 放射性活度在 0.029-0.386 Bq kg-1 之间（平均 = 0.197 ± 0.091 Bq kg-1，n = 14），其空间分布显示大亚湾入海口和西部的钚放射性活度相对较高，这主要归因于颗粒粒径较细。经证实，240Pu/239Pu 原子比值较高的原因是通过黑潮向太平洋核试验场（65% ± 7%）输送的钚。大亚湾核电站的正常运行没有释放额外的钚输入。此外，沉积岩芯的钚年代学显示，沉积环境的变化会影响钚的同位素含量。利用平流-扩散方程模型进一步评估和预测了大亚湾钚同位素的垂直迁移，表明钚随时间的扩散可能会影响其作为时间标记的作用。最后，我们为未来的环境风险评估提供了大亚湾钚同位素的基线值。

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来源期刊

ACS Earth and Space Chemistry Earth and Planetary Sciences-Geochemistry and Petrology

CiteScore

5.30

自引率

11.80%

发文量

249

期刊介绍： The scope of ACS Earth and Space Chemistry includes the application of analytical, experimental and theoretical chemistry to investigate research questions relevant to the Earth and Space. The journal encompasses the highly interdisciplinary nature of research in this area, while emphasizing chemistry and chemical research tools as the unifying theme. The journal publishes broadly in the domains of high- and low-temperature geochemistry, atmospheric chemistry, marine chemistry, planetary chemistry, astrochemistry, and analytical geochemistry. ACS Earth and Space Chemistry publishes Articles, Letters, Reviews, and Features to provide flexible formats to readily communicate all aspects of research in these fields.