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Title: Establishing rapid analysis of Pu isotopes in seawater to study the impact of Fukushima nuclear accident in the Northwest Pacific

Abstract

In order to evaluate the impact of the Fukushima derived Pu isotopes on seawater, a new analytical method to rapidly determine Pu isotopes in seawater by SF-ICP-MS including Fe(OH)2 primary co-precipitation, CaF2/LaF3 secondary co-precipitation and TEVA+UTEVA+DGA extraction chromatographic separation was established. High concentration efficiency (~100%) and high U decontamination factor (~107) were achieved. The plutonium chemical recoveries were 74–88% with the mean of 83 ± 5%. The precisions for both 240Pu/239Pu atom ratios and 239+240Pu activity concentrations were less than 5% when 15 L of seawater samples with the typical 239+240Pu activity of the Northwest Pacific were measured. It just needs 12 hours to determine plutonium using this new method. The limit of detection (LOD) for 239Pu and 240Pu were both 0.08 fg/mL, corresponding to 0.01 mBq/m3 for 239Pu and 0.05 mBq/m3 for 240Pu when a 15 L volume of seawater was measured. This method was applied to determine the seawater samples collected 446–1316 km off the FDNPP accident site in the Northwest Pacific in July of 2013. The obtained 239+240Pu activity concentrations of 1.21–2.19 mBq/m3 and the 240Pu/239Pu atom ratios of 0.198–0.322 implied that there was no significant Pu contamination from the accident to the Northwest Pacific.

Authors:
 [1]; ORCiD logo [2];  [3];  [2];  [2];  [4];  [2];  [2];  [5]
  1. National Inst. of Radiological Sciences (NIRS), Chiba (Japan); State Oceanic Administration, Xiamen (China)
  2. National Inst. of Radiological Sciences (NIRS), Chiba (Japan)
  3. National Inst. of Radiological Sciences (NIRS), Chiba (Japan); Univ. of South China, Hengyang (China)
  4. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
  5. Hirosaki Univ. (Japan)
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org.:
USDOE; China Scholarship Council; Ministry of Economy, Trade and Industry (METI) Japan
OSTI Identifier:
1548295
Grant/Contract Number:  
AC09-08SR22470
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY

Citation Formats

Men, Wu, Zheng, Jian, Wang, Hai, Ni, Youyi, Aono, Tatsuo, Maxwell, Sherrod L., Tagami, Keiko, Uchida, Shigeo, and Yamada, Masatoshi. Establishing rapid analysis of Pu isotopes in seawater to study the impact of Fukushima nuclear accident in the Northwest Pacific. United States: N. p., 2018. Web. doi:10.1038/s41598-018-20151-4.
Men, Wu, Zheng, Jian, Wang, Hai, Ni, Youyi, Aono, Tatsuo, Maxwell, Sherrod L., Tagami, Keiko, Uchida, Shigeo, & Yamada, Masatoshi. Establishing rapid analysis of Pu isotopes in seawater to study the impact of Fukushima nuclear accident in the Northwest Pacific. United States. doi:10.1038/s41598-018-20151-4.
Men, Wu, Zheng, Jian, Wang, Hai, Ni, Youyi, Aono, Tatsuo, Maxwell, Sherrod L., Tagami, Keiko, Uchida, Shigeo, and Yamada, Masatoshi. Tue . "Establishing rapid analysis of Pu isotopes in seawater to study the impact of Fukushima nuclear accident in the Northwest Pacific". United States. doi:10.1038/s41598-018-20151-4. https://www.osti.gov/servlets/purl/1548295.
@article{osti_1548295,
title = {Establishing rapid analysis of Pu isotopes in seawater to study the impact of Fukushima nuclear accident in the Northwest Pacific},
author = {Men, Wu and Zheng, Jian and Wang, Hai and Ni, Youyi and Aono, Tatsuo and Maxwell, Sherrod L. and Tagami, Keiko and Uchida, Shigeo and Yamada, Masatoshi},
abstractNote = {In order to evaluate the impact of the Fukushima derived Pu isotopes on seawater, a new analytical method to rapidly determine Pu isotopes in seawater by SF-ICP-MS including Fe(OH)2 primary co-precipitation, CaF2/LaF3 secondary co-precipitation and TEVA+UTEVA+DGA extraction chromatographic separation was established. High concentration efficiency (~100%) and high U decontamination factor (~107) were achieved. The plutonium chemical recoveries were 74–88% with the mean of 83 ± 5%. The precisions for both 240Pu/239Pu atom ratios and 239+240Pu activity concentrations were less than 5% when 15 L of seawater samples with the typical 239+240Pu activity of the Northwest Pacific were measured. It just needs 12 hours to determine plutonium using this new method. The limit of detection (LOD) for 239Pu and 240Pu were both 0.08 fg/mL, corresponding to 0.01 mBq/m3 for 239Pu and 0.05 mBq/m3 for 240Pu when a 15 L volume of seawater was measured. This method was applied to determine the seawater samples collected 446–1316 km off the FDNPP accident site in the Northwest Pacific in July of 2013. The obtained 239+240Pu activity concentrations of 1.21–2.19 mBq/m3 and the 240Pu/239Pu atom ratios of 0.198–0.322 implied that there was no significant Pu contamination from the accident to the Northwest Pacific.},
doi = {10.1038/s41598-018-20151-4},
journal = {Scientific Reports},
number = 1,
volume = 8,
place = {United States},
year = {2018},
month = {1}
}

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