Characteristic of Pu from urban wetland and lacustrine sediments in Suzhou Industrial Park, China
Introduction
Pu is an artificial radionuclide associated with nuclear industry including nuclear weapon and energy industry. Common anthropogenic Pu are in the form of 239Pu (T1/2 = 2.411 × 104 yr), 240Pu (T1/2 = 6563 yr), 241Pu (T1/2 = 14.4 yr), 242Pu (T1/2 = 3.73 × 105 yr) and 244Pu (T1/2 = 8.08 × 107 yr). Anthropogenic Pu in the environment mostly comes from the series of nuclear weapon tests from the mid-1940s to the 1980s. The atmospheric nuclear weapon tests conducted by countries such as the former Soviet Union, the United States and China have emitted about 1.1 × 1016Bq of 239+240Pu into the environment, and Pu was spread globally due to atmospheric dispersion (Harley, 1980).
The 240Pu/239Pu atom ratio differs for different sources such as nuclear test, military weapons or industrial sources. Therefore, the atom ratio is often used to identify the sources of radioactive pollutants in the environment (Krey et al., 1976; Warneke et al., 2002). Specifically, 240Pu/239Pu atom ratio of weapon-grade Pu ranges from 0.01–0.07 (Lindahl et al., 2017), while nuclear reactor-grade Pu exhibits higher atom ratios, ranging from 0.24–0.8 (Warneke et al., 2002; Ketterer and Szechenyi, 2008). Atom ratio values of the Pacific proving ground (PPG) Pu are usually 0.306–0.36, which are higher than the average value of 240Pu/239Pu atom ratios 0.1780.019 (0–30°N) and 0.1800.014 (30–71°N) from the global fallout (Krey et al., 1976; Kelley et al., 1999).
As 239Pu and 240Pu have a high radiotoxicity and long-term persistence in the environment, risk assessment for Pu in the environment is indispensable. More and more researchers are trying to determine the characteristics of distribution, sources and fate of Pu in different layers of the earth, including atmosphere, water and sediments (Hirose and Povinec, 2015; Zhang et al., 2018).
Regional studies on 239+240Pu activity concentration in the surface soils and its vertical distribution covers many part of China. However, 239+240Pu activities and inventories of the research areas are quite distinct from each other. The 239+240Pu activities in the surface soil range from 0.0230.003 mBq/g (Gansu, Lanzhou, northwestern China) to 1.300.05 mBq/g (Wuling, Chongqing, southwestern China) and the distinct 239+240Pu activities in China might be caused by the differences of soil particle sizes, organic matter, regional climatic factors and other factors (Zheng et al., 2009; Bu et al., 2014). In the vertical distribution of 239+240Pu, most Pu depositions (more than 80%) concentrate on the top 10 cm layer of soils (Dong et al., 2010; Bu et al., 2014). However, some soil core analyses show opposite results and the most Pu inventories are in the deeper layers (Zheng et al., 2009; Zhang and Hou, 2019) largely due to soil erosion and downward percolation of fine particles. Studies also show that the inventories of 239+240Pu in the estuary sediments are much larger than in soils, which might be caused by scavenging of Pu from the seawater and the higher sedimental deposition rates in the estuaries areas (Hao et al., 2018; Liu et al., 2011; Zhang et al., 2018).
The 240Pu/239Pu atom ratios have also been investigated in different regions and the results show that China has been affected by different sources of Pu and the global fallout is the main source of Pu in mainland (Huang et al., 2019). Studies have shown that the mainland of China, such as the northwest has been affected not only by the global fallout but also the Lop Nor nuclear tests conducted in the 1980s (Bu et al., 2015). Also, some results indicate that China coast including the marginal seas, such as the East China Sea, the Yellow Sea and the South China Sea, has been influenced by both the global fallout and the PPG (Pacific Proving Ground) close-in fallout (Dong et al., 2010; Liu et al., 2011, 2013; Wu et al., 2014; Zhang et al., 2018). It has been demonstrated that Pu derived from the PPG can be transported over long distances to the western Pacific Ocean and to its adjacent marginal seas (Liu et al., 2011; Wu et al., 2014). However, information on the distribution and characteristics of Pu deposition in the wetlands and lakes in the eastern China are very limited. Since China operates nuclear power plants (NPPs) along the east coast, investigating the historical deposition and migration mechanisms of Pu in urban wetlands and lakes is vitally important to understand and evaluate possible future pollution with radionuclides.
In this study, the spatial distributions of 239+240Pu activity of the urban wetlands in Suzhou Industrial Park (SIP) were measured for the first time and the sources of Pu in this area were investigated to see whether other sources such as Chinese nuclear tests or the Fukushima NPP accident have affected this area. In addition, a sediment core taken from Lake Yangcheng was also analyzed to investigate the historical information of Pu deposited in the lake.
Section snippets
Sample collection and preparation
The locations of the sampling sites are shown in Fig. 1. As seen in Fig. 1, the sample sites are distributed in Suzhou Industrial Park (SIP), Suzhou, eastern China. Suzhou (119°55′–121°20′ E, 30°47′–32°02′ N) is located in the middle of Yangtze River Delta and adjacent to Yangtze River and Lake Taihu. The city is under the impact of subtropical monsoon marine climate, having ~1100 mm annual precipitation.
Surface soil samples were collected in the wetlands of SIP in June 2012 (Fig. 1). The urban
239+240Pu activity concentration and its distribution in surface soils in Suzhou
The 239+240Pu activities and 240Pu/239Pu atom ratios in surface soil samples collected in SIP are presented in Table 1. The results show the activity concentration of 239+240Pu in the surface soil ranges from 0.035 to 0.426 mBq/g with the average value of 0.1560.08 mBq/g (arithmetic average) and 0.1260.013 mBq/kg (geometric average). The activity concentration values are close to the values (0.0880.031–0.4690.057 mBq/g) in Guangxi that Guan et al. (2018) reported. The maximum value of the
Conclusions
In this study, we analyzed 239+240Pu activities and 240Pu/239Pu atom ratios in surface soil samples and lacustrine sediment samples in Suzhou. The results indicate that the activity concentration of 239+240Pu from surface soil (0–4 cm) range from 0.035 to 0.426 mBq/g, with a mean of 0.1560.08 mBq/g. The 240Pu/239Pu atom ratio in surface soil samples ranged from 0.176 to 0.226, with a weighted mean of 0.194. The mean ratio was similar to the typical global fallout value. Using the Pearson
Declaration of competing interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgments
This work was supported by grants from the National Natural Science Foundation of China (41773004), the Jiangsu Provincial Key Laboratory of Radiation Medicine and Protection, the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).
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2022, Science of the Total EnvironmentCitation Excerpt :In this work, we study the surface and vertical distribution of 239+240Pu in soil samples collected in China and aim to: (1) systematically investigate the surface and vertical distribution characterization of 239+240Pu in Chinese soil samples based on all the publicly available surface and core sample data in China; (2) summarize the mean 240Pu/239Pu atom ratio and source identification based on statistical analysis; and (3) provide the migration parameters of 239+240Pu for the CDE model in Chinese soil cores, which can be served as an important reference for harmful heavy metal migration and soil risk assessment research. This study evaluates 239+240Pu surface soil data from 647 samples sites (see more information in Tables S1 and S2; see sample locations in Fig. 1) in China collected from published papers (Sha et al., 1991; Kelley et al., 1999; Jin et al., 2003; Huh and Su, 2004; Zheng et al., 2009; Dong et al., 2010a; Dong et al., 2010b; Dong, 2010; Liu et al., 2013; Bu and Guo, 2013; Wang et al., 2013; Xu et al., 2013; Bu et al., 2014; Bu et al., 2015; Xing, 2015; Yu et al., 2017; Xu et al., 2017; Bu et al., 2017; Guan et al., 2018; Xing et al., 2018; Zhang et al., 2018; Ni et al., 2018; Cao et al., 2019; Zhang et al., 2019; Zhang and Hou, 2019; Wu, 2019; Zhuang et al., 2019; Ni et al., 2020; Wang et al., 2020; Guan et al., 2020; Zhao et al., 2020; Guan et al., 2021; Dang et al., 2021; Zhang et al., 2021). The definition of the surface layer soil depth is not the same across different articles (see more information in Tables S1 and S2).
Rapid determination of plutonium isotopes in small samples using single anion exchange separation and ICP-MS/MS measurement in NH<inf>3</inf>–He mode for sediment dating
2022, TalantaCitation Excerpt :These values were at least one order of magnitude lower than those (from 0.012 ± 0.012 mBq/g to 1.698 ± 0.210 mBq/g) obtained in the sediments from the Lake Yangcheng [30], which is < 100 km far from the Lake Ge. However, the 240Pu/239Pu atomic ratios in the sediment core of the Lake Ge ranging from 0.137 ± 0.033 to 0.220 ± 0.047 with an average of 0.171 ± 0.016, generally fell in the range of the global fallout values [31] and also agreed well with the results (the 240Pu/239Pu atomic ratios with an average of 0.174) measured in the Lake Yangcheng [30]. This indicated that Pu in the Lake Ge should also be mainly from the global fallout.
Distribution of plutonium isotopes in soils between two nuclear test sites: Semipalatinsk and Lop Nor
2022, Journal of Environmental RadioactivityDistribution and source identification of Pu in the tidal flat wetlands of northern Jiangsu Province and radial sand ridge of southern Yellow Sea-An explanation of “land-sea interaction”
2021, CatenaCitation Excerpt :These samples maybe received PPG close-in fallout Pu from the currents from the south of the ECS. Compared with the previous study results, most of the 240Pu/239Pu atom ratios in our study were consistent with the ratios in the soils of China (0.19) (e.g. Dong et al., 2010; Lindahl et al., 2011; Bu et al., 2014, 2015, 2018; Xing, 2015; Xu et al., 2017; Zhang et al., 2018; Xing et al., 2018; Huang, 2019; Guan et al., 2018, 2020), which indicated that the Pu in our samples was from the global fallout. While the 240Pu/239Pu atom ratios in our study samples were lower compared with the ratios in the samples of China Seas, both seawater and sediment, except for samples in the northern Yellow Sea (~0.18) (Xu et al., 2018) and the Liaodong Bay (0.173–0.241) (Zhuang et al., 2019).