南海环境中Pu、Np的清除机制和空间迁移模拟研究
PDF下载 (154)刘志勇,韦小敏.南海环境中Pu、Np的清除机制和空间迁移模拟研究[J].宁波大学学报(理工版),2024,37(4):41-47.DOI:10.20098/j.cnki.1001-5132.2024.0107
LIU Zhiyong,WEI Xiaomin.Discussion of scavenging mechanism and spatial migration simulation for Pu and Np in South China Sea[J].Journal of Ningbo University(Natural Science & Engineering Edition),2024,37(4):41-47.DOI:10.20098/j.cnki.1001-5132.2024.0107
| Title: | Discussion of scavenging mechanism and spatial migration simulation for Pu and Np in South China Sea |
| 作者: | 刘志勇, 韦小敏 |
| Author(s): | LIU Zhiyong, WEI Xiaomin |
| 关键词: | 中国南海; Pu、Np; 迁移和扩散; 清除过程; 模型模拟 |
| Keywords: | South China Sea; Pu and Np; migration and diffusion; scavenging process; model simulation |
| 分类号: | P736.4 |
| DOI: | 10.20098/j.cnki.1001-5132.2024.0107 |
| 文献标识码: | A |
| 摘要: | 海洋环境中Pu、Np两种放射性元素源自人类核活动. 由于洋流、海陆交汇等多重效应导致Pu、Np被富集于边缘海区域, 威胁人类的环境安全. 目前国内外对海洋中Pu、Np的研究未成体系, 研究方法多局限于含量分析. 为研究河流输入量、地形、气候等因素对于海洋中Pu、Np清除效率的影响, 本文采用扇形磁场高分辨率质谱(SF-ICP-MS)对南海水体、沉积物中的Pu、Np比活度, 240Pu/239Pu和237Np/239Pu原子比进行精确分析. 在模拟海洋生态环境和顺序提取实验基础上, 研究Pu、Np在海洋中的扩散问题. 根据得到的Pu、Np比活度和同位素原子比等在水体、颗粒物以及沉积物中的分布数据, 拟合得到Pu、Np在南海传输和扩散的特征关键参数, 以解释南海海水中Pu、Np的清除机制. 最后利用数据构建南海Pu、Np空间迁移与清除的稳态模型(S-ADE), 后续将通过模拟及现场取样分析对模型进行相互校验. 研究结果可为核事故中Pu、Np等放射性污染物的溯源与迁移的快速分析与综合评估, 以及放射性污染防护与治理提供方案. |
| Abstract: | Pu and Np are radioactive elements in marine environments, derived from human nuclear activities. They are enriched in marginal sea areas due to the multi-effect caused by ocean currents, and land-sea interaction, which threatens people’s nuclear environment safety. However, there is no systematic research on Pu and Np in the ocean in China and abroad, and the research method is limited to concentration analyses. In order to study the influence of runoff input, terrain, climate, and other factors on the scavenging efficiency of Pu and Np, this paper uses sector field inductively coupled plasma mass spectrometry (SF-ICP-MS) to accurately analyze the activities of Pu and Np, as well as the atomic ratios of 240Pu/239Pu and 237Np/239Pu in seawaters and sediments of the South China Sea. The diffusion of Pu and Np in the ocean was studied on the basis of a simulated marine environment experiment and a sequential extraction experiment. The key parameters describing the transmission characteristics and migration/diffusion of Pu and Np in the seawater of the South China Sea were obtained by fitting the content and isotope atomic ratios distribution data of Pu and Np in water, particulate matter, and sediment to explain the scavenging mechanism of the Pu and Np in the seawater of South China Sea. Finally, according to the obtained data, a dynamic simulation model (S-ADE) of the spatial distribution and scavenging mechanisms of Pu, Np in the South China Sea was established, and the cross-validation of the model was carried out by experimental and field sample analyzing data. The study can provide solutions for the rapid analysis and comprehensive assessment of the origin and migration of Pu, Np and other radioactive pollutants in nuclear accidents, as well as for the protection and management of radioactive contamination. |
| 参考文献 /References: | [1] MALARA G, ZEMA D A, ARENA F, et al. Coupling watershed-coast systems to study evolutionary trends: a review[J]. Earth-Science Reviews, 2020, 201:103040. [2] TAN Karsoon, CAI X H, TAN Kianann, et al. A review of natural and anthropogenic radionuclide pollution in marine bivalves[J]. The Science of the Total Environment, 2023, 896:165030. [3] United Nations Scientific Committee on the Effect of Atomic Radiation. Sources, effects and risks of ionizing radiation[EB/OL]. [2023-12-10]. https://www.unscear. org/unscear/en/publications/2020_2021_1.html. [4] HIROSE K, POVINEC P P. Ten years of investigations of Fukushima radionuclides in the environment: a review on process studies in environmental compartments[J]. Journal of Environmental Radioactivity, 2022, 251/252: 106929. [5] TOSCANO-JIMENEZ M, GARIC R, TENORIO A. Modelling the dispersion of 137Cs in marine ecosystems with Monte Carlo methods[J]. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, 2004, 213:779- 783. [6] YAMADA M, ZHENG J. Enhanced boundary scavenging of 241Am on the continental margin of the East China Sea[J]. Journal of Environmental Radioactivity, 2022, 255:107044. [7] PERIÁÑEZ R, SUH K S, MIN B I. The behaviour of 137Cs in the North Atlantic Ocean assessed from numerical modelling: releases from nuclear fuel reprocessing factories, redissolution from contaminated sediments and leakage from dumped nuclear wastes[J]. Marine Pollution Bulletin, 2016, 113:343-361. [8] WU J W, DAI M H, XU Y, et al. Sources and accumulation of plutonium in a large Western Pacific marginal sea: the South China Sea[J]. Science of the Total Environment, 2018, 610/611:200-211. [9] HAN X X, ZHU J J, ZHU Y W, et al. 237Np and 241Am as fingerprints in the major river basins of Southern China and North South China Sea: a land-sea perspective[J]. ACS Omega, 2021, 6:26897-26909. [10] ZHANG M T, HOU X L, ZHANG L Y, et al. Distribution of anthropogenic 129I in the western South China Sea and its application for tracing the sources and movement of pollution[J]. Environmental Science & Technology, 2022, 56(17):12298-12306. [11] ZHANG F L, WANG J L, LIU D T, et al. Distribution of 137Cs in the Bohai Sea, Yellow Sea and East China Sea: sources, budgets and environmental implications[J]. The Science of the Total Environment, 2019, 672:1004-1016. [12] LIU Z F, ZHAO Y L, COLIN C C, et al. Source- to-sink transport processes of fluvial sediments in the South China Sea[J]. Earth-Science Reviews, 2016, 153:238- 273. [13] BENEDIK L, TRDIN M. Determination of low level Np-237 by various techniques[J]. Applied Radiation and Isotopes, 2017, 126:208-213. [14] SNOW M S, MORRISON S S, CLARK S B, et al. 237Np analytical method using 239Np tracers and application to a contaminated nuclear disposal facility[J]. Journal of Environmental Radioactivity, 2017, 172:89-95. [15] HUANG Z, HOU X L, ZHAO X. Rapid and simultaneous determination of 238Pu, 239Pu, 240Pu, and 241Pu in samples with high-level uranium using ICP-MS/ MS and extraction chromatography[J]. Analytical Chemistry, 2023, 95(34):12931-12939. [16] MACSIK Z, LAMONT S P, MAASSEN J R, et al. Radioanalytical method for the separation of trace plutonium and neptunium from uranium[EB/OL]. [2023- 12-10]. https://link.springer.com/article/10.1007/s10967- 024-09360-6. [17] HUANG Z, HOU X L, QIAO J X, et al. Simultaneous determination of femtogram levels of 237Np, 239Pu, and 240Pu in environmental solid samples using extraction chromatography and ICP-MS/MS[J]. Talanta, 2023, 265: 124798. [18] MONTGOMERY D A, MARTINEZ N E. Dosimetric modeling of Tc-99, Cs-137, Np-237, and U-238 in the grass species Andropogon virginicus: development and comparison of stylized, voxel, and hybrid phantom geometry[J]. Journal of Environmental Radioactivity, 2020, 211:106075. [19] CAI Z Y, CHEN D K, GAN J P. Formation of the layered circulation in South China Sea with the mixing stimulated exchanging current through Luzon strait[J]. JGR Oceans, 2023, 128(3):e2023JC019730. [20] SANTSCHI P H, XU C, ZHANG S, et al. Iodine and plutonium association with natural organic matter: a review of recent advances[J]. Applied Geochemistry, 2017, 85:121-127. [21] GRASER C H, BANIK N L, BENDER K A, et al. Sensitive redox speciation of iron, neptunium, and plutonium by capillary electrophoresis hyphenated to inductively coupled plasma sector field mass spectrometry [J]. Analytical Chemistry, 2015, 87(19):9786-9794. [22] WEI X M, ZHANG R H, ZHU J J, et al. Spatial distribution and modelling of 239+240Pu in the sediments and seawater columns of the South China Sea and Indian Ocean[J]. Environmental Pollution, 2024, 343:123244. [23] XIE T X, DAI M H, HAMZAH F, et al. Sources and transport of plutonium in the Indo-Pacific intersection: implications for South China Sea freshwater transport into Indonesian Seas[J]. Chemical Geology, 2021, 580: 120367. |
| 备注/Memo: | 收稿日期: 2024−01−05. 宁波大学学报（理工版）网址: http://journallg.nbu.edu.cn/ 基金项目: 国家自然科学基金（42373006）. 第一作者: 刘志勇, 博士/教授, 主要研究方向: 同位素地球化学及环境放射化学. E-mail: liuzy@suda.edu.cn 宁波大学学报（理工版）网址：http://journallg.nbu.edu.cn/ |
