中国东部海域中<sup>239+240</sup>Pu的来源与沉积过程研究

黄亚楠

doi:10.12284/hyxb2022123

中国东部海域中^239+240Pu的来源与沉积过程研究

doi: 10.12284/hyxb2022123

黄亚楠^{1, 2,}

1.
中山大学海洋科学学院，广东珠海 519082
2.
西班牙国家加速器中心，安达卢西亚自治区塞维利亚 41092

基金项目: 广东省青年优秀人才国际培养计划博士后项目（20210616）

详细信息

作者简介:
黄亚楠（1986-），男，河南省正阳县人，助理研究员，从事同位素地球化学与年代学研究。E-mail: huangyn69@mail.sysu.edu.cn

中图分类号: P736.4⁺4
计量
- 文章访问数: 560
- HTML全文浏览量: 137
- PDF下载量: 65
- 被引次数: 0
出版历程
- 收稿日期: 2021-11-19
- 修回日期: 2022-05-01
- 网络出版日期: 2022-06-23
- 刊出日期: 2022-11-03

Source and sedimentary process of ^239+240Pu in the eastern China seas

Huang Ya’nan^{1, 2
,}

1.
School of Marine Science, Sun Yat-sen University, Zhuhai 519082, China
2.
Centro Nacional de Aceleradores, Sevilla 41092, Spain

摘要

摘要: 本文对东海及毗邻海域中^239+240Pu比活度、²⁴⁰Pu/²³⁹Pu原子比值和^239+240Pu累积通量或沉积通量数据进行整理，首次从大气沉降、海水中、生物体中、沉积物捕获器中以及沉积物中的^239+240Pu 5个方面阐述了东海及毗邻海域中^239+240Pu的地球化学行为。研究结果表明，全球大气沉降和太平洋核试验场输入的^239+240Pu是东海海水和沉积物中^239+240Pu的两个主要来源；在长江径流、浙闽沿岸流、台湾暖流、黑潮与上升流等水团的混合作用以及清除作用的影响下，东海近岸海水中^239+240Pu浓度在时间上呈现被清除而减少的趋势，相应近岸浅水区沉积物中^239+240Pu的埋藏深度高于远岸深水海域。在黑潮入侵和上升流的作用下，冲绳海槽区尤其是台湾岛东北部，沉积物中的^239+240Pu比活度与沉积通量显著增大。同时，利用东海表层沉积物中^239+240Pu比活度和²⁴⁰Pu/²³⁹Pu原子比值的相关关系证实了台湾东北部黑潮底层分支流的存在，并指示出台湾暖流与黑潮底层分支流可能交汇的海域位置。
- ^239+240Pu /
- ²⁴⁰Pu/²³⁹Pu /
- 东海 /
- 沉积物 /
- 海水
Abstract: This study compiled the data of ^239+240Pu specific activity, ²⁴⁰Pu/²³⁹Pu atom ratio and ^239+240Pu flux or inventory in the East China Sea and adjacent waters. Based on the ^239+240Pu concentration in atmospheric fallout, ^239+240Pu in seawater, ^239+240Pu in organisms,^239+240Pu in sediment trap and ^239+240Pu in sediment, the geochemical behavior of ^239+240Pu were explained in the East China Sea and adjacent waters. The results showed that global fallout and Pacific proving grounds close-in fallout were the two major sources of ^239+240Pu. Under the influence of water masses such as the Changjing River diluted water, Zhejiang-Fujian Coastal Current, Taiwan Warm Current, Kuroshio Current and upwelling current, mixing effect and removal effect, the concentration of ^239+240Pu in coastal waters of the East China Sea showed a trend of removal over time, the burial depth of ^239+240Pu in the near shore sediments was deeper than that in the far sea area. In the northeast of Taiwan Island of China, the ^239+240Pu specific activity and ^239+240Pu inventory in Okinawa Trough increased significantly under the influence of Kuroshio current intrusion and upwelling current. At the same time, this study found that the relationship between ^239+240Pu specific activity and ²⁴⁰Pu/²³⁹Pu atom ratio in surface sediments of the East China Sea, and confirmed the existence of a tributary of the Kuroshio bottom in northeastern Taiwan, and indicated the location where the Taiwan Warm Current and a tributary of the Kuroshio bottom may intersect.
- ^239+240Pu /
- ²⁴⁰Pu/²³⁹Pu /
- East China Sea /
- sediment /
- seawater

HTML全文

图 1 东海及毗邻区^239+240Pu样品的采集站位（海流根据文献[3]改绘）

Fig. 1 The sites of ^239+240Pu samples in the East China Sea and adjacent waters (current modified from reference [3])

下载: 全尺寸图片幻灯片

图 2 全球预测地表空气与日本城市中^239+240Pu的浓度^[22]

Fig. 2 The concentrations of ^239+240Pu in surface air form globally predicted and Japanese cities^[22]

下载: 全尺寸图片幻灯片

图 3 东海及毗邻区表层海水中^239+240Pu浓度与²⁴⁰Pu/²³⁹Pu随时间的变化

Fig. 3 Changes of ^239+240Pu concentration and ²⁴⁰Pu/²³⁹Pu in surface water of the East China Sea and adjacent waters over time

下载: 全尺寸图片幻灯片

图 4 水柱中^239+240Pu浓度的分布特征^{[7, 12]}

Fig. 4 Distribution of ^239+240Pu concentration in different water columns^{[7, 12]}

下载: 全尺寸图片幻灯片

图 5 长鳍金枪鱼组织中²³⁹Pu比活度的变化^[28]

Fig. 5 Changes of the ²³⁹Pu specific activity in Thunnus alalunga tissues^[28]

下载: 全尺寸图片幻灯片

图 6 比较不同深度海水中^239+240Pu比活度和累积通量时间序列^{[9, 29]}

Fig. 6 Compare the specific activity and flux time series of ^239+240Pu specific activity in seawater at different depths^{[9, 29]}

下载: 全尺寸图片幻灯片

图 7 东海及毗邻区表层沉积物中^239+240Pu比活度与²⁴⁰Pu/²³⁹Pu的相关关系

Fig. 7 The relationship between ^239+240Pu specific activity and ²⁴⁰Pu/²³⁹Pu in surface sediments of the East China Sea and adjacent waters

下载: 全尺寸图片幻灯片

图 8 东海及毗邻区沉积物柱样中^239+240Pu比活度的分布特征^{[15-16, 20]}

Fig. 8 Vertical Distributions of ^239+240Pu specific activity in sediment cores of the East China Sea and adjacent waters^{[15-16, 20]}

下载: 全尺寸图片幻灯片

表 1 东海及毗邻区^239+240Pu样品的数据信息

Tab. 1 Data information about ^239+240Pu samples in the East China Sea and adjacent waters

序号	^239+240Pu样品类型	个数	测定方法	标样验证	采样时间	参考资料
1	海水（表层）	10*	α能谱	n.a.	1981年	文献[6]
2	沉积物（表层）+海水（表层）	31	α能谱	n.a.	1971–1996年	MARIS
3	海水（柱样）+沉积物（柱样）	10	α能谱	n.a.	1987年前后	文献[7−8]
4	沉积物（柱样）	22	α能谱	IAEA-SD-N-1	1998年之前	文献[2]
5	悬浮颗粒物+沉积物（柱样）	5	α能谱	n.a.	1991年11月	文献[9]
6	沉积物（柱样）	34	α能谱	IAEA-SD-N-1	1996–1999年	文献[10]
7	生物体（中华哲水蚤）	1	α能谱	n.a.	1993–1996年	文献[11]
8	海水（表层）	22	α能谱	n.a.	1993–1996年	文献[1]
9	海水（柱样）	3	α能谱	n.a.	1993年10月	文献[12]
10	海水（表层）	16	α能谱	n.a.	1993–1994年	文献[13]
11	沉积物（柱样）	6	ICP-MS	IAEA-133A,327,375	2000–2003年	文献[14]
12	沉积物（柱样）	6	ICP-MS	IAEA-368	1992–1995年	文献[15]
13	沉积物（柱样）	1	AMS	colAMS	2006年4月	文献[16]
14	沉积物（表层样+柱样）	21	SF-ICP-MS	IAEA-368	2006年4月	文献[17]
15	沉积物（表层样+柱样）	29	ICP-MS X-II	IAEA-376	2013年8月	文献[18]
16	海水（表层）	7	ICP-MS	IAEA-384，395，443	2011年，2014–2015年	文献[19]
17	沉积物（表层样+柱样）	48	SF-ICP-MS	IAEA-368	2013–2015年	文献[20]
18	沉积物（表层样）	8	SF-ICP-MS	IAEA-368	2019年之前	文献[21]
注：*表示每个站位有2个平行样取平均值；n.a.表示从原文中无法获得；（）内表示具体的样品类型；MARIS表示海洋放射性核素信息系统（Marine Radioactivity Information System），参见https://maris.iaea.org/。

下载: 导出CSV

参考文献(34)

[1]	Lee S H, Gastaud J, Povinec P P, et al. Distribution of plutonium and americium in the marginal seas of the Northwest Pacific Ocean[J]. Deep-Sea Research Part II: Topical Studies in Oceanography, 2003, 50(17/21): 2727−2750.
[2]	Huh C A, Su C C. Sedimentation dynamics in the East China Sea elucidated from ²¹⁰Pb, ¹³⁷Cs and ^239+240Pu[J]. Marine Geology, 1999, 160(1/2): 183−196.
[3]	王建丰, 司广成, 于非. 台湾暖流变化特征及机制研究进展[J]. 海洋科学, 2020, 44(5): 141−148. Wang Jianfeng, Si Guangcheng, Yu Fei. Progress in studies of the characteristics and mechanisms of variations in the Taiwan warm current[J]. Marine Sciences, 2020, 44(5): 141−148.
[4]	UNSCEAR. Sources, effects of ionizing radiation[M]//Unscear. Report to the General Assembly with Annex B. New York: United Nations, 2000.
[5]	黄亚楠, 潘少明. 中国边缘海柱样沉积物中^239+240Pu的分布与时标价值[J]. 中国环境科学, 2020, 40(3): 1235−1245. doi: 10.3969/j.issn.1000-6923.2020.03.035 Huang Ya’nan, Pan Shaoming. The dating and distribution of ^239+240Pu in the sediment cores of the marginal sea of China[J]. China Environmental Science, 2020, 40(3): 1235−1245. doi: 10.3969/j.issn.1000-6923.2020.03.035
[6]	李培泉, 颜启民, 于银亭. 冲绳海槽及东海表层海水中超铀元素钚的测定[J]. 海洋科学, 1988(3): 43−46. Li Peiquan, Yan Qimin, Yu Yinting. The determination of plutonium in surface seawater of Okinawa Trough and East China Sea[J]. Marine Sciences, 1988(3): 43−46.
[7]	Nagaya Y, Nakamura K. ^{239, 240}Pu and ¹³⁷Cs in the East China and the Yellow Seas[J]. Journal of Oceanography, 1992, 48(1): 23−35. doi: 10.1007/BF02234030
[8]	Yamada M, Zheng Jian. Determination of ²⁴⁰Pu/²³⁹Pu atom ratio in seawaters from the East China Sea[J]. Radiation Protection Dosimetry, 2011, 146(1/3): 311−313.
[9]	Yamada M, Aono T. Large particle flux of ^239+240Pu on the continental margin of the East China Sea[J]. Science of the Total Environment, 2002, 287(1/2): 97−105.
[10]	Su C C, Huh C A. ²¹⁰Pb, ¹³⁷Cs and ^{239, 240}Pu in East China Sea sediments: sources, pathways and budgets of sediments and radionuclides[J]. Marine Geology, 2002, 183(1/4): 163−178.
[11]	Hong G H, Kim Y I, Lee S H, et al. ^239+240Pu and ¹³⁷Cs concentrations for zooplankton and nekton in the Northwest Pacific and Antarctic Oceans (1993−1996)[J]. Marine Pollution Bulletin, 2002, 44(7): 660−665. doi: 10.1016/S0025-326X(01)00322-8
[12]	Yamada M, Aono T. Vertical profiles of ^239+240Pu in seawater from the East China Sea[J]. Journal of Radioanalytical and Nuclear Chemistry, 2003, 256(3): 399−402. doi: 10.1023/A:1024579111492
[13]	Hong G H, Chung C S, Lee S H, et al. Artificial radionuclides in the Yellow Sea: Inputs and redistribution[J]. Radioactivity in the Environment, 2006, 8: 96−133.
[14]	Lee S Y, Huh C A, Su C C, et al. Sedimentation in the southern Okinawa Trough: enhanced particle scavenging and teleconnection between the Equatorial Pacific and western Pacific margins[J]. Deep-Sea Research Part I: Oceanographic Research Papers, 2004, 51(11): 1769−1780. doi: 10.1016/j.dsr.2004.07.008
[15]	Wang Zhongliang, Yamada M. Plutonium activities and ²⁴⁰Pu/²³⁹Pu atom ratios in sediment cores from the East China Sea and Okinawa Trough: sources and inventories[J]. Earth and Planetary Science Letters, 2005, 233(3/4): 441−453.
[16]	Tims S G, Pan Shaoming, Zhang R, et al. Plutonium AMS measurements in Yangtze River Estuary sediment[J]. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, 2010, 268(7/8): 1155−1158.
[17]	Liu Zhiyong, Zheng Jian, Pan Shaoming, et al. Pu and ¹³⁷Cs in the Yangtze River Estuary sediments: distribution and source identification[J]. Environmental Science & Technology, 2011, 45(5): 1805−1811.
[18]	Wang Jinlong, Baskaran M, Hou Xiaolin, et al. Historical changes in ²³⁹Pu and ²⁴⁰Pu sources in sedimentary records in the East China Sea: implications for provenance and transportation[J]. Earth and Planetary Science Letters, 2017, 466: 32−42. doi: 10.1016/j.jpgl.2017.03.005
[19]	Wu Junwen. Sources and scavenging of plutonium in the East China Sea[J]. Marine Pollution Bulletin, 2018, 135: 808−818. doi: 10.1016/j.marpolbul.2018.08.014
[20]	Zhang Rui, Wang Ruirui, Liu Zhiyong, et al. Distribution and transport of plutonium in the sediments of the Yangtze River Estuary and the adjacent East China Sea[J]. Applied Geochemistry, 2020, 115: 104532. doi: 10.1016/j.apgeochem.2020.104532
[21]	Liu Zhiyong, Hu Jun, Yamada M, et al. Uranium and plutonium isotopes and their environmental implications in surface sediments from the Yangtze River catchment and estuary[J]. Catena, 2020, 193: 104605. doi: 10.1016/j.catena.2020.104605
[22]	Thakur P, Khaing H, Salminen-Paatero S. Plutonium in the atmosphere: a global perspective[J]. Journal of Environmental Radioactivity, 2017, 175−176: 39−51. doi: 10.1016/j.jenvrad.2017.04.008
[23]	张克新, 潘少明, 徐仪红, 等. 长江口放射性核素Pu的大气湿沉降初步研究[J]. 地理科学, 2016, 36(1): 157−160. doi: 10.13249/j.cnki.sgs.2016.01.020 Zhang Kexin, Pan Shaoming, Xu Yihong, et al. Atmospheric wet deposition of radionuclide Pu in the Changjiang River Estuary region[J]. Scientia Geographica Sinica, 2016, 36(1): 157−160. doi: 10.13249/j.cnki.sgs.2016.01.020
[24]	Yamada M, Zheng Jian. ²⁴⁰Pu/²³⁹Pu atom ratios in water columns from the North Pacific Ocean and Bering Sea: transport of Pacific proving grounds-derived Pu by ocean currents[J]. Science of the Total Environment, 2020, 718: 137362. doi: 10.1016/j.scitotenv.2020.137362
[25]	Wu Junwen, Dai Minhan, Xu Yi, 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. doi: 10.1016/j.scitotenv.2017.07.226
[26]	Imai T, Sakanoue M. Content of plutonium, thorium and protactinium in sea water and recent coral in the North Pacific[J]. Journal of the Oceanographical Society of Japan, 1973, 29(2): 76−82.
[27]	Buesseler K O. The isotopic signature of fallout plutonium in the North Pacific[J]. Journal of Environmental Radioactivity, 1997, 36(1): 69−83. doi: 10.1016/S0265-931X(96)00071-9
[28]	Folsom T R. Several measurements of global radioactive fallout-speculation of the characteristics of the North Pacific that control the rate of dispersion of certain surface pollutants[J]. Isotope Ocean Chemistry, 1990: 30−72.
[29]	Yamada M, Aono T. ²³⁸U, Th isotopes, ²¹⁰Pb and ^239+240Pu in settling particles on the continental margin of the East China Sea: fluxes and particle transport processes[J]. Marine Geology, 2006, 227(1/2): 1−12.
[30]	黄亚楠, 潘少明, 刘志勇. 中国边缘海沉积物中^239+240Pu 的来源与存量模型[J]. 地理科学, 2018, 38(11): 1892−1903. Huang Ya’nan, Pan Shaoming, Liu Zhiyong. The source and inventory model of in the sediment cores of the marginal sea of China[J]. Scientia Geographica Sinica, 2018, 38(11): 1892−1903.
[31]	Yang Dezhou, Yin B aoshu, Liu Zhiliang, et al. Numerical study of the ocean circulation on the East China Sea shelf and a Kuroshio bottom branch northeast of Taiwan in Summer[J]. Journal of Geophysical Research Atmospheres, 2011, 116(C5): C05015.
[32]	李安春, 张凯棣. 东海内陆架泥质沉积体研究进展[J]. 海洋与湖沼, 2020, 51(4): 705−727. doi: 10.11693/hyhz20200500145 Li Anchun, Zhang Kaidi. Research progress of mud wedge in the inner continental shelf of the East China Sea[J]. Oceanologia et Limnologia Sinica, 2020, 51(4): 705−727. doi: 10.11693/hyhz20200500145
[33]	Pittauer D, Roos P, Qiao Jixin, et al. Pacific proving grounds radioisotope imprint in the Philippine Sea sediments[J]. Journal of Environmental Radioactivity, 2018, 186: 131−141. doi: 10.1016/j.jenvrad.2017.06.021
[34]	Huang Ya’nan, Sun Xiaoming, Zhang Wei, et al. Spatial distribution and migration of ^239+240Pu in Chinese soils[J]. Science of the Total Environment, 2022, 824: 153724. doi: 10.1016/j.scitotenv.2022.153724