Journal of Soils and Sediments

, Volume 19, Issue 1, pp 491–500 | Cite as

Migration path and isotope tracing of 137Cs and 239 + 240Pu in estuary sediments: a case study of Liao River estuary in China

  • Kexin ZhangEmail author
  • Guosheng Li
  • Shaoming Pan
  • Xiaoqing Qian
  • Zhiyong Liu
  • Yihong Xu
  • Yongpei Hao
Sediments, Sec 3 • Hillslope and River Basin Sediment Dynamics • Research Article



Currently, the distribution characteristics and transport processes of the radionuclides 137Cs and 239 + 240Pu in the sediments of estuaries are still a controversial issue. Thus, in the present study, we investigated the distribution characteristics, sources and migration path of 137Cs and 239 + 240Pu in sediment cores of the Liao River estuary (LRE), China, and evaluated the relative contributions of the Pacific Proving Grounds (PPG) and riverine sources of Pu for the sediments in this area. We used 137Cs and Pu isotopes for dating the sediments and estimated the sedimentation rates by the two radionuclides in the LRE.

Materials and methods

Seven sediment samples were collected using a box corer from the Liao River estuarine wetland and tidal flat in the LRE in October 2012 and April 2015, respectively. The activities of 137Cs in the various samples were determined by γ spectrometry using HP-Ge detectors with 60% relative counting efficiency. Approximately 2–5 g of sediment were spiked with 242Pu (ca. 1 mBq) as a chemical yield tracer for Pu isotopic analysis at the School of Radiation Medicine and Protection, Soochow University. The measurement of Pu isotopes (239Pu, 240Pu, 242Pu) was performed by a sector field ICP-MS. In order to quantitatively differentiate the relative proportions of global fallout and PPG, we employed a two-end member mixing model to estimate their contributions.

Results and discussion

The average values of 137Cs, 239 + 240Pu activity concentrations, and 240Pu/239Pu atom ratios in the surface sediment samples of the LRE were 6.727 ± 0.251 mBq g−1, 0.294 ± 0.024 mBq g−1, and 0.188 ± 0.049 (1σ), respectively. The average 240Pu/239Pu atom ratios ranged from 0.180 ± 0.034 to 0.199 ± 0.021 in sediment cores from the east and west sides of the LRE. For core LT-2 values for 137Cs and 239 + 240Pu concentrations were from below the detection limit: 3.380 ± 0.414 and 0.036 ± 0.007 to 0.105 ± 0.007 mBq g−1. The mean 240Pu/239Pu atom ratio 0.217 ± 0.050 (1σ) in sediment core LT-2 lies between the global fallout and PPG close-in fallout.


We found that atmospheric fallout is the main source of Pu in sediment cores from the east and west sides of the LRE. For core LT-2, atmospheric fallout and riverine input (~ 73.4%) are the major sources of Pu with the source of the rest of Pu (~ 26.6%) attributed to the PPG via the Tsushima Warm Current and the coastal water of the East China Sea. The sedimentation rates (means 0.62–0.8 cm year−1) estimated by the two radionuclides were in good agreement and without any statistically significant difference.


137Cs Isotope tracing Liao River estuary Migration path Plutonium 



We are very grateful to the anonymous reviewers and the editor of this journal for their constructive comments in the manuscript.

Funding information

This work was supported by the China Postdoctoral Science Foundation (Nos. 2017M611922, 2018T110559), the Natural Science Foundation of Jiangsu Province (No. BK20171292), the Postdoctoral Science Foundation of Jiangsu Province (No. 1701186B), and the National Natural Science Foundation of China (Nos. 41501286, 41671466).


  1. Baskaran M, Asbill S, Santschi P, Brooks J, Champ M, Adkison D, Colmer MR, Makeyev V (1996) Pu, 137Cs and excess 210Pb in Russian Artic sediments. Earth Planet Sci Lett 140:243–257CrossRefGoogle Scholar
  2. Bu WT, Zheng J, Guo QJ Aono T, Tazoe H, Tagami K, Uchida S, Yamada M (2014) A method of measurement of 239Pu, 240Pu, 241Pu in high U content marine sediments by sector field ICP-MS and its application to Fukushima sediment samples. Environ Sci Technol 48:534–541CrossRefGoogle Scholar
  3. Buesseler KO (1997) The isotopic signature of fallout plutonium in the North Pacific. J Environ Radioact 36:69–83CrossRefGoogle Scholar
  4. Cao LG, Zheng J, Tsukata H, Pan SM, Wang ZT, Tagammi K, Uchida S (2016) Simultaneous determination of radiocesium (135Cs, 137Cs) and plutonium (239Pu, 240Pu) in river suspended particles by ICP-MS/MS and SF-ICP-MS. Talanta 159:55–63CrossRefGoogle Scholar
  5. Dai MH, Buesseler KO, Kelley JM, Andrews JE, Pike S, Wacker JF (2001) Size-fractionated plutonium isotopes in a coastal environment. J Environ Radioact 53:9–25CrossRefGoogle Scholar
  6. Dai MH, Kelley JM, Buesseler KO (2002) Sources and migration of plutonium in groundwater at the Savannah River site. Eviron Sci Technol 36:3690–3699CrossRefGoogle Scholar
  7. Hancock GJ, Leslie C, Everett SE Tims SG, Brunskill GJ, Haese R (2011) Plutonium as a chronomarker in Australian and New Zealand sediments: a comparison with 137Cs. J Environ Radioact 102:919–929CrossRefGoogle Scholar
  8. Harley JH (1980) Plutonium in the environment-a review. J Radiat Res 21:83–104CrossRefGoogle Scholar
  9. Hirose K, Sugimura Y (1990) Plutonium isotopes in the surface air in Japan: effect of Chernobyl accident. J Radioanal Nucl Chem 138:127–138CrossRefGoogle Scholar
  10. Hirose K, Igarashi Y, Aoyama M (2008) Analysis of the 50-year records of the atmospheric deposition of long-lived radionuclides in Japan. Appl Radiat Isotopes 66:1675–1678CrossRefGoogle Scholar
  11. Huh CA, Su CC (1999) Sedimentation dynamics in the East China Sea elucidated from 210Pb, 137Cs and 239,240Pu. Mar Geol 160:183–196CrossRefGoogle Scholar
  12. Kelley JM, Bond LA, Beasley TM (1999) Global distribution of Pu isotopes and 237Np. Sci Total Environ 237-238:483–500CrossRefGoogle Scholar
  13. Kershaw PJ, Woodhead DS Lovett MB, Leonard KS (1995) Plutonium from European reprocessing operations—its behavior in the marine environment. Appl Radiat Isotopes 46:1121–1134CrossRefGoogle Scholar
  14. Ketterer ME, Hafera KM, Jonesb VJ, Appleby PG (2004) Rapid dating of recent sediments in Loch Ness: inductively coupled plasma mass spectrometric measurements of global fallout plutonium. Sci Total Environ 322:221–229CrossRefGoogle Scholar
  15. Kim CK, Kim CS, Chang BU Choi SW, Chung CS, Hong GH, Hirose K, Igarashi Y (2004) Plutonium isotopes in seas around the Korean Peninsula. Sci Total Environ 318:197–209CrossRefGoogle Scholar
  16. Koide M, Bertine KK, Chow TJ, Goldberg ED (1985) The 240Pu/239Pu ratio, a potential geochronometer. Earth Planet Sci Lett 72:1–8CrossRefGoogle Scholar
  17. Krey PW (1976) Remote plutonium contamination and total inventories from Rocky flats. Health Phys 30:209–214Google Scholar
  18. Lee SY, Gastaud J, Povinec PP, Hong GH, Kim SH, Chung CS, Lee KW, Pettersson HBL (2003) Distribution of plutonium and americium in the marginal seas of the northwest Pacific Ocean. Deep-Sea Res II 50:2727–2750CrossRefGoogle Scholar
  19. Lee SY, Huh CA, Su CC, You CF (2004) Sedimentation in the Southern Okinawa Trough: enhanced particle scavenging and teleconnection between the Equatorial Pacific and western Pacific margins. Deep-Sea Res I Oceanogr Res Pap 51:1769–1780CrossRefGoogle Scholar
  20. Leslie C, Hancock GJ (2008) Estimating the date corresponding to the horizon of the first detection of 137Cs and 239+240Pu in sediment cores. J Environ Radioact 99:483–490CrossRefGoogle Scholar
  21. Liao HQ, Bu WT, Zheng J, Wu FC, Yamada M (2014) Vertical distributions of radionuclides (239+240Pu, 240Pu/239Pu and 137Cs) in sediment cores of Lake Bosten in Northwestern China. Environ Sci Technol 48:3840–3846CrossRefGoogle Scholar
  22. Lind OC, Oughton DH, Salbu B, Skipperud L, Sickel MA, Brown JE, Fifield LK, Tims SG (2006) Transport of low 240Pu/239Pu atom ratio plutonium- species in the Ob and Yenisey Rivers to the Kara Sea. Earth Planet Sci Lett 251:33–43CrossRefGoogle Scholar
  23. Lindahl P, Lee SH, Worsfold P, Keit-Roach M (2010) Plutonium isotopes as tracers for ocean processes: a review. Mar Environ Res 69:73–84CrossRefGoogle Scholar
  24. Lindahl P, Worsfold P, Keith-Roach M, Andersen MB, Kershaw P, Leonard K, Choi MS, Boust D, Lesueur P (2011) Temporal record of Pu isotopes in inter-tidal sediments from the northeastern Irish Sea. Sci Total Environ 409:5020–5025CrossRefGoogle Scholar
  25. Liu ZY, Zheng J, Pan SM, Dong W, Yamada M, Aono T, Guo QJ (2011) Pu and 137Cs in the Yangtze River estuary sediments: distribution and source identification. Eviron Sci Technol 45:1805–1811CrossRefGoogle Scholar
  26. Liu ZY, Zheng J, Pan SM, Gao JH (2013) Anthropogenic plutonium in the North Jiangsu tidal flats of the Yellow Sea in China. Environ Monit Assess 185:3807–3817Google Scholar
  27. Livingston HD, Povinec PP (2002) A millennium perspective on the contribution of global fallout radionuclides to ocean science. Health Phys 82:656–668CrossRefGoogle Scholar
  28. Martin JM, Thomas AJ (1990) Origins, concentrations and distributions of artificial radionuclides discharged by the Rhône River to the Mediterranean Sea. J Environ Radioact 11:105–139CrossRefGoogle Scholar
  29. Muramatsu Y, Hamilton T, Uchida S, Tagami K, Yoshida S, Robison W (2001) Measurement of 240Pu/239Pu isotopic rations in the soil from the Marshall Islands using ICP-MS. Sci Total Environ 278:151–159CrossRefGoogle Scholar
  30. Nagaya Y, Nakamura K (1992) 239,240Pu and 137Cs in the East China and the yellow seas. J Oceanogr 48:23–25CrossRefGoogle Scholar
  31. Olsen CR, Thein M, Larsen IL, Lowry PD, Mulholland PJ, Cutshall NH, Byrd JT, Windom HL (1989) Plutonium, lead-210, and carbon isotopes in the Savannah estuary: river borne versus marine sources. Eviron Sci Technol 23:1475–1481CrossRefGoogle Scholar
  32. Pan SM, Tims SG, Liu XY, Fifield LK (2011) 137Cs, 239+240Pu concentrations and the 240Pu/239Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary. J Environ Radioact 102:930–936CrossRefGoogle Scholar
  33. Sholkovitz ER (1983) The geochemistry of plutonium in fresh and marine water environments. Earth-Sci Rev 19:95–161CrossRefGoogle Scholar
  34. Song YX, Zhan XW, Wang YG (1997) The modern sedimentary characters in the northern of the Liaodong Bay. Acta Oceanol Sin 19:145–149Google Scholar
  35. Su JL, Yuan LY (2005) The hydrology of the coastal waters in China. Ocean Press, Beijing, pp 145–162Google Scholar
  36. Tims SG, Pan SM, Zhang R, Fifield LK, Wang YP, Gao JH (2010) Plutonium AMS measurements in Yangtze River estuary sediment. Nucl Instrum Meth B 268:1155–1158CrossRefGoogle Scholar
  37. UNSCEAR (2000) Sources and effects of Ionizing radiation; United nations scientific committee on the effects of atomic radiation exposures to the public from manmade sources of radiation. United Nations, New YorkGoogle Scholar
  38. Wang ZL, Yamada M (2005) Plutonium activities and 240Pu/239Pu atom ratios in sediment cores from the East China Sea and Okinawa Trough: sources and inventories. Earth Planet Sci Lett 233:441–453CrossRefGoogle Scholar
  39. Wang JL, Baskaran M, Hou XL, Du JZ, Zheng J (2017) Historical changes in 239Pu and 240 Pu sources in sedimentary records in the East China Sea: implications for provenance and transportation. Earth Planet Sci Lett 466:32–42CrossRefGoogle Scholar
  40. Warneke T, Croudace IW, Warwick PE, Taylor RN (2002) A new ground-level fallout record of uranium and plutonium isotopes for northern temperate latitudes. Earth Planet Sci Lett 203:1047–1057CrossRefGoogle Scholar
  41. Wu FC, Zheng J, Liao HQ, Yamada M (2010) Vertical distributions of plutonium and 137Cs in lacustrine sediments in northwestern China: quantifying sediment accumulation rates and source identifications. Environ Sci Technol 44:2911–2917CrossRefGoogle Scholar
  42. Wu JW, Zheng J, Dai MH, Huh CA, Chen WF, Tagami K, Uchida S (2014) Isotopic composition and distribution of plutonium in northern South China Sea sediments revealed continuous release and transport of Pu from the Marshall Islands. Environ Sci Technol 48:3136–3144CrossRefGoogle Scholar
  43. Xu YH, Qiao JX, Hou XL, Pan SM (2013) Plutonium isotopes in soils from Northeast China and its potential application for evaluation of soil erosion. Sci Rep 3:3506Google Scholar
  44. Xu YH, Qiao JX, Pan SM, Hou XL, Roos P, Cao LG (2015) Plutonium as a tracer for soil erosion assessment in Northeast China. Sci Total Environ 511:176–185Google Scholar
  45. Yamada M, Zheng J, Wang ZL (2006) 137Cs, 239+240Pu and 240Pu/239Pu atom ratios in the surface waters of the Western North Pacific Ocean, Eastern Indian Ocean and their adjacent seas. Sci Total Environ 366:242–252CrossRefGoogle Scholar
  46. Zheng J, Yamada M (2004) Sediment core record of global fallout and bikini close-in fallout Pu in Sagami Bay, Western Northwest Pacific Margin. Environ Sci Technol 38:498–504Google Scholar
  47. Zheng J, Yamada M (2006a) Inductively coupled plasma-sector field mass spectrometry with a high-efficiency sample introduction system for the determination of Pu isotopes in settling particles at femtogram levels. Talanta 69:1246–1253CrossRefGoogle Scholar
  48. Zheng J, Yamada M (2006b) Plutonium isotopes in settling particles: transport and scavenging of Pu in the western Northwest Pacific. Environ Sci Technol 40:4103–4108CrossRefGoogle Scholar
  49. Zheng J, Wu FC, Yamada M, Liao HQ, Liu CQ, Wan GJ (2008) Global fallout Pu recorded in lacustrine sediments in Lake Hongfeng, SW China. Environ Pollut 152:314–321CrossRefGoogle Scholar
  50. Zheng J, Tagami K, Watanabe Y, Uchida S, Aono T, Ishii N, Yoshida S, Kubota Y, Fuma S, Ihara S (2012) Isotopic evidence of plutonium release into the environment from the Fukushima DNPP accident. Sci Rep 2:304CrossRefGoogle Scholar
  51. Zhu LH, Wu JZ, Hu RJ (2009) Geomorphological evolution of the Liaohe River delta in recent 20 years. Acta Geograph Sin 64:357–367Google Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  • Kexin Zhang
    • 1
    • 2
    • 3
    Email author
  • Guosheng Li
    • 4
  • Shaoming Pan
    • 2
  • Xiaoqing Qian
    • 1
  • Zhiyong Liu
    • 5
  • Yihong Xu
    • 2
  • Yongpei Hao
    • 2
  1. 1.College of Environmental Science and EngineeringYangzhou UniversityYangzhouChina
  2. 2.The Key Laboratory of Coastal and Island Development of Ministry of Education, School of Geographic and Oceanographic SciencesNanjing UniversityNanjingChina
  3. 3.Yangzhou Hongshuo Environmental and Biological Engineering Research Co. Ltd.YangzhouChina
  4. 4.Institute of Geographic Sciences and Natural Resources ResearchCASBeijingChina
  5. 5.School of Radiation Medicine and ProtectionSoochow UniversitySuzhouChina

Personalised recommendations