skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Fukushima Daiichi reactor source term attribution using cesium isotope ratios from contaminated environmental samples

Journal Article · · Rapid Communications in Mass Spectrometry
DOI:https://doi.org/10.1002/rcm.7468· OSTI ID:1251624
 [1];  [1];  [1]
  1. Idaho National Lab. (INL), Idaho Falls, ID (United States)

Source term attribution of environmental contamination following the Fukushima Daiichi Nuclear Power Plant (FDNPP) disaster is complicated by a large number of possible similar emission source terms (e.g. FDNPP reactor cores 1–3 and spent fuel ponds 1–4). Cesium isotopic analyses can be utilized to discriminate between environmental contamination from different FDNPP source terms and, if samples are sufficiently temporally resolved, potentially provide insights into the extent of reactor core damage at a given time. In this work, rice, soil, mushroom, and soybean samples taken 100–250 km from the FDNPP site were dissolved using microwave digestion. Radiocesium was extracted and purified using two sequential ammonium molybdophosphate-polyacrylonitrile columns, following which 135Cs/137Cs isotope ratios were measured using thermal ionization mass spectrometry (TIMS). Results were compared with data reported previously from locations to the northwest of FDNPP and 30 km to the south of FDNPP. 135Cs/137Cs isotope ratios from samples 100–250 km to the southwest of the FDNPP site show a consistent value of 0.376 ± 0.008. 135Cs/137Cs versus 134Cs/137Cs correlation plots suggest that radiocesium to the southwest is derived from a mixture of FDNPP reactor cores 1, 2, and 3. Conclusions from the cesium isotopic data are in agreement with those derived independently based upon the event chronology combined with meteorological conditions at the time of the disaster. In conclusion, cesium isotopic analyses provide a powerful tool for source term discrimination of environmental radiocesium contamination at the FDNPP site. For higher precision source term attribution and forensic determination of the FDNPP core conditions based upon cesium, analyses of a larger number of samples from locations to the north and south of the FDNPP site (particularly time-resolved air filter samples) are needed. Published in 2016. This article is a U.S. Government work and is in the public domain in the USA.

Research Organization:
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Sponsoring Organization:
US Department of Homeland Security (DHS); USDOE Office of Nuclear Energy (NE); USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
AC07-05ID14517; 2012-DN-130-NF0001-02
OSTI ID:
1251624
Alternate ID(s):
OSTI ID: 1358431
Report Number(s):
INL/JOU-15-35648
Journal Information:
Rapid Communications in Mass Spectrometry, Vol. 30, Issue 4; ISSN 0951-4198
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 29 works
Citation information provided by
Web of Science

References (28)

Evaluation of Radioactive Contamination Caused by Each Plant of Fukushima Daiichi Nuclear Power Station Using 134Cs/137Cs Activity Ratio as an Index [134Cs/137Cs放射能比を指標とした福島第一原子力発電所事故に由来する放射性核種の放出原子炉別汚染評価] journal January 2013
Preliminary Estimation of Release Amounts of 131 I and 137 Cs Accidentally Discharged from the Fukushima Daiichi Nuclear Power Plant into the Atmosphere journal July 2011
Concentrations of 137Cs and 40K in Mushrooms Consumed in Japan and Radiation Dose as a Result of Their Dietary Intake journal January 2004
Preliminary evaluation of 135Cs/137Cs as a forensic tool for identifying source of radioactive contamination journal January 2008
First retrieval of hourly atmospheric radionuclides just after the Fukushima accident by analyzing filter-tapes of operational air pollution monitoring stations journal October 2014
Resuspension: Decadal Monitoring Time Series of the Anthropogenic Radioactivity Deposition in Japan journal January 2003
COMPARISON OF 241Am, 239,240Pu AND 137Cs CONCENTRATIONS IN SOIL AROUND ROCKY FLATS journal January 1999
Xenon-133 and caesium-137 releases into the atmosphere from the Fukushima Dai-ichi nuclear power plant: determination of the source term, atmospheric dispersion, and deposition journal January 2012
Method for ultra-trace cesium isotope ratio measurements from environmental samples using thermal ionization mass spectrometry journal May 2015
Radioactive cesium isotope ratios as a tool for determining dispersal and re-dispersal mechanisms downwind from the Nevada Nuclear Security Site journal August 2012
Anthropogenic Radionuclides in Japanese Food: Environmental and Legal Implications journal February 2013
Mechanical environmental transport of actinides and 137Cs from an arid radioactive waste disposal site journal October 2015
137 Cs Activities and 135 Cs/ 137 Cs Isotopic Ratios from Soils at Idaho National Laboratory: A Case Study for Contaminant Source Attribution in the Vicinity of Nuclear Facilities journal February 2015
Analysis of a Nuclear Accident: Fission and Activation Product Releases from the Fukushima Daiichi Nuclear Facility as Remote Indicators of Source Identification, Extent of Release, and State of Damaged Spent Nuclear Fuel journal August 2012
Concentration and specific activity of fallout 137Cs in extracted and particle-size fractions of cultivated soils journal June 2008
Radiocesium concentrations in mushrooms collected in Japan journal January 1994
Post-Accident Sporadic Releases of Airborne Radionuclides from the Fukushima Daiichi Nuclear Power Plant Site other January 2015
Post-Accident Sporadic Releases of Airborne Radionuclides from the Fukushima Daiichi Nuclear Power Plant Site journal November 2015
135Cs/137Cs isotopic composition of environmental samples across Europe: Environmental transport and source term emission applications journal January 2016
Analysis of cesium isotope compositions in environmental samples by thermal ionization mass spectrometry – 1. A preliminary study for source analysis of radioactive contamination in Fukushima prefecture: Fukushima NPP Accident Related Paper journal March 2014
Determination of radioactive cesium isotope ratios by triple quadrupole ICP-MS and its application to rainwater following the Fukushima Daiichi Nuclear Power Plant accident journal January 2014
Transfer of 137Cs and stable Cs from paddy soil to polished rice in Aomori, Japan journal January 2002
Variations of 137Cs depositions and soil concentrations between alpine and montane soils in northern Colorado journal January 2000
Characterization of spent fuel approved testing material---ATM-105 report December 1991
Heavy element radionuclides (Pu, Np, U) and 137Cs in soils collected from the Idaho National Engineering and Environmental Laboratory and other sites in Idaho, Montana, and Wyoming report October 1998
Accumulation of radiocesium in basidiomycetes collected from Japanese forests journal December 1994
135 Cs/ 137 Cs Isotopic Ratio as a New Tracer of Radiocesium Released from the Fukushima Nuclear Accident journal May 2014
Xenon-133 and caesium-137 releases into the atmosphere from the Fukushima Dai-ichi nuclear power plant: determination of the source term, atmospheric dispersion, and deposition journal January 2011

Cited By (10)

Ultra-trace determination of the 135 Cs/ 137 Cs isotopic ratio by thermal ionization mass spectrometry with application to Fukushima marine sediment samples journal January 2019
Provenance of uranium particulate contained within Fukushima Daiichi Nuclear Power Plant Unit 1 ejecta material journal June 2019
The role of mass spectrometry in radioactive contamination assessment after the Fukushima nuclear accident journal January 2018
Spatial pattern of plutonium and radiocaesium contamination released during the Fukushima Daiichi nuclear power plant disaster journal November 2018
Environmental nuclear forensics: the need for a new scientific discipline journal May 2019
135Cs activity and 135Cs/137Cs atom ratio in environmental samples before and after the Fukushima Daiichi Nuclear Power Plant accident journal April 2016
Provenance of uranium particulate contained within Fukushima Daiichi Nuclear Power Plant Unit 1 ejecta material text January 2019
Isotopic signature and nano-texture of cesium-rich micro-particles: Release of uranium and fission products from the Fukushima Daiichi Nuclear Power Plant journal July 2017
Isotopic ratios of uranium and caesium in spherical radioactive caesium-bearing microparticles derived from the Fukushima Dai-ichi Nuclear Power Plant journal February 2020
Analysis of External Surface Irregularities on Fukushima-Derived Fallout Particles journal September 2017