90Sr in marine environment: Comparison of seas surrounding Japan and the South China Sea
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摘要: 90Sr长期被视为最重要的人工放射性核素之一，日本福岛核事故导致包括90Sr在内的大量放射性物质泄漏进入海洋，厂区储水罐中冷却废水至今仍然存在大量90Sr。海洋中90Sr分析方法却繁琐耗时，导致核事故后的90Sr研究较为匮乏，且缺乏系统的认识。本研究在2015−2018年期间测量南海海水和多种海洋生物(马尾藻、海虾、牡蛎、红树林植物、造礁珊瑚)中90Sr的基础上，深入分析核事故后日本周边海域和南海90Sr的比活度水平与环境半衰期。结合文献资料，本研究发现1975−2010年期间日本近岸海水90Sr的环境半衰期为15.4 a，2011年的核事故后日本周边海洋中90Sr比活度显著升高，基于ERICA软件定量计算核事故后90Sr对海洋鱼类的剂量率比核事故前的结果高5个数量级。南海作为福岛核事故后北太平洋环流的下游海域，本文进一步构建1984−2018年期间南海90Sr比活度的历史曲线，发现核事故前后南海90Sr比活度水平没有可识别的变化，进一步定量计算南海90Sr的环境半衰期为26.7 a，发现边缘海和大洋中90Sr和137Cs环境半衰期格局差异与核素(90Sr和137Cs)的源汇过程(河流输入和海洋生物泵)密切相关。鉴于海洋中90Sr分析方法的挑战性，本文发现在10多种海洋生物中造礁珊瑚骨骼几乎拥有最高的90Sr浓集因子(约1 000 L/kg)，同时具有较易大量获取、固定附着生长、连续高分辨率记录、前处理简单快速等优点，很可能是海洋中90Sr可靠的指示生物。造礁珊瑚中90Sr研究将有利于揭示人工放射性核素的源汇过程，同时为我国海洋放射性监测方案和相关标准导则的优化和完善提供有益的参考。Abstract: 90Sr is recognized to be one of most important artificial radionuclides. A huge amount of radioactive substance (e.g., 90Sr) was released into marine environment after the Fukushima Nuclear Accident (FNA). High 90Sr activity was still observed in the treated wastewater which was stored on site in many tanks. However, 90Sr was rarely investigated in marine environment due to its complicated and time-consuming analytical procedure after the FNA, constraining a comprehensive understanding of the fate of 90Sr in marine environment. We discussed the 90Sr activity and environmental half-life (EHL) in seas surrounding Japan (SSJ) and the South China Sea (SCS) on the basis of previous data and our 90Sr data in seawater and marine biotas (e.g., sargassum, shrimp, oyster, mangrove, reef coral) collected from the SCS during 2015−2018. We found that the EHL of 90Sr in the SSJ was 15.4 years during 1975−2010. 90Sr in the SSJ was significantly elevated after the FNA. Radiation dose rate of 90Sr on marine fish was increased by five orders of magnitude after the FNA relative to the baseline before the FNA. As the downstream basin of the North Pacific Subtropical Gyre, the SCS was not identified with noticeable 90Sr-derived from the FNA. The EHL of 90Sr in the SCS was calculated to be 26.7 years during 1984−2018 based on the compilation of historical 90Sr data. The contrasting patterns of the EHL of 90Sr and 137Cs in the marginal seas and open oceans were attributed to the distinct sources (river input) and sinks (marine biological pump) of 90Sr and 137Cs. In the context of challenge of 90Sr analytical method in marine environment, extremely high 90Sr concentration factor (around 1000 L/kg) was observed in the reef coral skeleton after comparing with concentration factors of 90Sr in more than 10 kinds of marine biotas. Additionally, reef coral is potential to be a reliable 90Sr marine bioindicator with other advantages of easy availability in large quantity, growth at a fixed location, continue record with high resolution, and simple pretreatment. The study of 90Sr in reef coral will not only help to reveal distinct sources and sinks of artificial radionuclides in marine environment, but also provide valuable insights to optimization and improvement of standards/guidelines of marine radioactivity monitoring program.
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Key words:
- Fukushima Nuclear Accident /
- radioactivity /
- seawater /
- biotas /
- sediment /
- reef coral
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图 2 1965−2018年日本周边海域的海水90Sr比活度的历史曲线
Fig. 2 Historical 90Sr activity in seawater from the sea surrounding Japan during 1965−2018
图 3 1984−2018年期间南海海水90Sr的历史变化曲线
Fig. 3 Historical 90Sr activity in seawater from the South China Sea during 1984−2018
表 1 福岛核事故后日本周边海域的海水中90Sr的比活度
Tab. 1 90Sr activity in seawater from the sea surrounding Japan after the Fukushima Nuclear Accident
样品来源 年份 位置 比活度范围/Bq·m−3 平均值/Bq·m−3 参考文献 福岛核电站附近海水 2011 37.40°N, 141.20°E 200.00～4.00×105 − [5] 福岛外海海水(15 km外) 2011 37.50°N, 141.20°E 10.00～9.00×103 − [5] 日本近海海水样品 2011 34.00～38.00°N,141.00～148.00°E 0.80～85.00 − [10] 福岛核电站附近海水 2011 36.25～41.10°N,141.00～141.20°E 6.00～104.00 − [42] 2012 36.25～41.10°N,141.00～141.20°E 2.00～53.00 − [42] 2013 36.25～41.10°N,141.00～141.20°E 3.00～42.00 − [42] 福岛核电站附近海水 2013 36.60～37.60°N,141.00～141.50°E 0.66～29.13 6.66 [43] 福岛核电站附近海水 2013 37.40°N,141.10°E 154.20～172.30 160.20 [44] 福岛核电站附近海水 2013 37.00～38.37°N,141.02～141.50°E 0.60～8.90 − [12] 福岛核电站附近海水 2014 37.43°N,141.04°E − 26.00 [45] 福岛核电站附近海水 2015 37.43°N,141.04°E − 1.53 [45] 福岛核电站附近海水 2016 37.43°N,141.04°E − 1.03 [45] 注：−表示参考文献并未给出具体数据。 
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表 2 福岛核事故后日本周边海域的海洋沉积物中90Sr比活度
Tab. 2 90Sr activity in marine sediment from the sea surrounding Japan after the Fukushima Nuclear Accident
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表 3 福岛核事故后日本周边海域的海洋生物中90Sr的比活度
Tab. 3 90Sr activity in marine biotas from the sea surrounding Japan after the Fukushima Nuclear Accident
样品来源 年份 经纬度 比活度范围/Bq·kg−1 平均值/Bq·kg−1 参考文献 福岛核电站港湾内海洋鱼类 2013 37.40°N, 141.00°E <170.00 − [57] 福岛外海海洋鱼类 2011−2014 37.20～37.50°N,140.90～141.20°E <1.20 − [15] 海洋贝类 2011 36.25～41.10°N，141.00～141.20°E 0.13×10−1～1.91×10−1 − [42] 2012 36.25～41.10°N，141.00～141.20°E 0.29×10−1 ～0.85×10−1 − [42] 2013 37.40°N,141.00°E 0.57×10−1 0.57×10−1 [42] 西北太平洋海洋生物 2012 − 0.01～0.19 − [17] 注：−表示参考文献并未给出具体数据。
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表 4 基于ERICA软件的核事故前后90Sr对海洋鱼类的电离辐射评价
Tab. 4 ERICA tool-derived radiation dose rate of 90Sr on marine fish in pre-Fukushima and post-Fukushima eras
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表 5 海洋生物中90Sr比活度与浓集因子
Tab. 5 90Sr activity and its concentration factor in marine biotas
海洋生物种类 90Sr比活度/Bq·kg−1 浓集因子/L·kg−1 参考文献 南海造礁珊瑚骨骼 1.21 ～1.00×103 [79] 福岛核事故后的海洋双壳类软组织 0.01～0.17 ～1.40 [42] 福岛核事故后的西北太平洋鱿鱼 0.02～0.05 4.00～19.00 [17] 福岛核事故后的西北太平洋海洋鱼类 0.01～0.06 3.00～49.00 [17] 波罗的海海洋鱼类（比目鱼） 鱼骨 0.77 81.80 [59] 波罗的海海洋鱼类（比目鱼） 肌肉 0.06 8.40 [59] 波罗的海海洋鱼类（比目鱼） 全鱼 0.16 25.40 [59] 波罗的海海洋双壳类 0.57～1.19 61.00～129.00 [56] 广西防城港核电站周边海虾 0.06～0.07 28.00～40.00 本研究 广西防城港核电站周边牡蛎 0.18 75.00 本研究 广西防城港核电站周边马尾藻 0.10 45.00 本研究 广西防城港核电站周边红树林 0.20～0.50 106.00～217.00 本研究 有孔虫 − 150.00 [80] 颗石藻 − 320.00 [81] 双壳类外壳 − 250.00 [82] 鱼类耳石 − 500.00 [83] 仙掌藻 − 1.10×103 [84] 注：−表示参考文献中没有90Sr的数据，浓集因子基于元素Sr浓度计算获得。
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