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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]
+ Show Author Affiliations
  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.
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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. https://doi.org/10.1038/s41598-018-20151-4
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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. https://doi.org/10.1038/s41598-018-20151-4. https://www.osti.gov/servlets/purl/1548295.
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@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 = {Tue Jan 30 00:00:00 EST 2018},
month = {Tue Jan 30 00:00:00 EST 2018}
}
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https://doi.org/10.1038/s41598-018-20151-4
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Ultra-trace determination of plutonium in marine samples using multi-collector inductively coupled plasma mass spectrometry
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Rapid method for the determination of 226Ra in hydraulic fracturing wastewater samples
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Determination of plutonium isotopes in waters and environmental solids: A review
journal, October 2009

Ultra-trace determination of plutonium in marine samples using multi-collector inductively coupled plasma mass spectrometry
journal, June 2010

  • Lindahl, Patric; Keith-Roach, Miranda; Worsfold, Paul
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  • DOI: 10.1016/j.aca.2010.05.012

Determination of 237Np and Pu isotopes in large soil samples by inductively coupled plasma mass spectrometry
journal, December 2010

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  • Analytica Chimica Acta, Vol. 682, Issue 1-2
  • DOI: 10.1016/j.aca.2010.10.001

No Fukushima Dai-ichi derived plutonium signal in marine sediments collected 1.5–57 km from the reactors
journal, November 2017

Spatial and temporal distribution of Pu in the Northwest Pacific Ocean using modern coral archives
journal, April 2012

240Pu/239Pu atom ratios in seawater from Sagami Bay, western Northwest Pacific Ocean: sources and scavenging
journal, December 2007

137Cs, 239+240Pu concentrations and the 240Pu/239Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary
journal, October 2011

Plutonium isotopes concentration in seawater and bottom sediment off the Pacific coast of Aomori sea area during 1991–2005
journal, March 2011

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239Pu and 240Pu inventories and 240Pu/239Pu atom ratios in the equatorial Pacific Ocean water column
journal, July 2012

Plutonium determination in seawater by inductively coupled plasma mass spectrometry: A review
journal, May 2016

Measurement of 240Pu/239Pu isotopic ratios in soils from the Marshall Islands using ICP-MS
journal, October 2001

The isotopic signature of fallout plutonium in the North Pacific
journal, January 1997

Determination of Pu Isotopes in Seawater by an On-Line Sequential Injection Technique with Sector Field Inductively Coupled Plasma Mass Spectrometry
journal, August 2002

  • Kim, Cheol-Su; Kim, Chang-Kyu; Lee, Kun Jai
  • Analytical Chemistry, Vol. 74, Issue 15
  • DOI: 10.1021/ac0255328

Sequential Injection Method for Rapid and Simultaneous Determination of 236 U, 237 Np, and Pu Isotopes in Seawater
journal, November 2013

  • Qiao, Jixin; Hou, Xiaolin; Steier, Peter
  • Analytical Chemistry, Vol. 85, Issue 22
  • DOI: 10.1021/ac402673p

Pu and 137 Cs in the Yangtze River Estuary Sediments: Distribution and Source Identification
journal, March 2011

  • Liu, Zhiyong; Zheng, Jian; Pan, Shaoming
  • Environmental Science & Technology, Vol. 45, Issue 5
  • DOI: 10.1021/es1035688

Release of Plutonium Isotopes into the Environment from the Fukushima Daiichi Nuclear Power Plant Accident: What Is Known and What Needs to Be Known
journal, August 2013

  • Zheng, Jian; Tagami, Keiko; Uchida, Shigeo
  • Environmental Science & Technology, Vol. 47, Issue 17
  • DOI: 10.1021/es402212v

Rapid Multisample Analysis for Simultaneous Determination of Anthropogenic Radionuclides in Marine Environment
journal, March 2014

  • Qiao, Jixin; Shi, Keliang; Hou, Xiaolin
  • Environmental Science & Technology, Vol. 48, Issue 7
  • DOI: 10.1021/es404584b

Isotopic evidence of plutonium release into the environment from the Fukushima DNPP accident
journal, March 2012

  • Zheng, Jian; Tagami, Keiko; Watanabe, Yoshito
  • Scientific Reports, Vol. 2, Issue 1
  • DOI: 10.1038/srep00304

Determination of Pu isotope concentrations and isotope ratio by inductively coupled plasma mass spectrometry: a review of analytical methodology
journal, January 2007

  • Kim, Cheol-Su; Kim, Chang-Kyu; Martin, Paul
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Heavy Isotope Abundances in Mike Thermonuclear Device
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Plutonium Isotopes Concentration in Seawater along the Algerian Coast
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Pu Distribution in Seawater in the Near Coastal Area off Fukushima after the Fukushima Daiichi Nuclear Power Plant Accident
journal, January 2015

  • Bu, W. T.; Zheng, J.; Aono, T.
  • Journal of Nuclear and Radiochemical Sciences, Vol. 15, Issue 1
  • DOI: 10.14494/jnrs.15.1_1

Distribution of Pu isotopes in marine sediments in the Pacific 30 km off Fukushima after the Fukushima Daiichi nuclear power plant accident
journal, January 2012

Isotopic determination of U, Pu and Cs in environmental waters following the Fukushima Daiichi Nuclear Power Plant accident
journal, January 2012

  • Sakaguchi, Aya; Kadokura, Akinobu; Steier, Peter
  • GEOCHEMICAL JOURNAL, Vol. 46, Issue 4
  • DOI: 10.2343/geochemj.2.0216
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