Determination of isotopic composition of plutonium in hot particles of the Chernobyl area

Boulyga, Sergei F.; Erdmann, N.; Funk, H.; Kievets, M.K.; Lomonosova, E.M.; Mansel, A.; Trautmann, Ν.; Yaroshevich, O.I.; Zhuk, I.V.

doi:10.1016/s1350-4487(97)00098-x

Cited by 47 publications

(14 citation statements)

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“…Overall, the analyzed micro-sample entity ( n = 48) showed a variation from low to high Pu isotope ratios, ranging from 0.007(2) to 0.047(8) for 242 Pu/ 239 Pu and from 0.183(13) to 0.577(40) for 240 Pu/ 239 Pu. It should be noted that very limited data are provided in the literature regarding the Pu isotopic composition of individual particles collected in the vicinity of the accidental Chernobyl reactor [ 36 , 37 ]. Thus, no information about the Pu isotopic distribution has been available so far for the Chernobyl fallout.…”

Section: Resultsmentioning

confidence: 99%

“… Soil ( n = 8) ICP-MS Boulyga and Becker [ 43 ] 0.396(14) a n.a. Soil ( n = 8) ICP-MS Nunnemann et al [ 24 ] 0.394(2) b 0.027(1) b Soil ( n = 1) RIMS Erdmann et al [ 25 ] 0.378(2) a,b 0.024(1) a,b Soil RIMS Boulyga et al [ 36 ] 0.329(16) b 0.021(3) b Hot particle ( n = 1) RIMS Wendt et al [ 37 ] 0.378(2) b 0.088(1) b Hot particle ( n = 1) RIMS Kirchner and Noack [ 46 ] 0.56 a,c 0.044 a,c Reactor core Calculation Begichev et al [ 47 ] 0.39 a,c 0.045 a,c Reactor core Calculation This study 0.388(86) a 0.028(11) a Fuel particle clusters ( n = 48) LA-MC-ICP-MS This study 0.183(13) to 0.577(40) 0.007(2) to 0.047(8) Fuel particle clusters ( n = 48) LA-MC-ICP-MS a Average values b Isotope ratios were calculated from published isotopic compositions c Isotope ratios were calculated from published activity data …”

Section: Resultsmentioning

confidence: 99%

“…A modified multi-collector set-up allowed to measure ultra-trace Pu isotope amounts, whereas the use of laser ablation sampling allowed to determining variations of the Pu isotopic composition both between and within individual fuel particle cluster samples. Up to now, only a very limited amount of data has been available for individual hot particle samples from the Chernobyl fallout [ 36 , 37 ]. Since, in this study, a large number of individual particle cluster samples ( n = 48) were analyzed and spatially resolved for the Pu isotopic composition, important insights are provided for the first time about the distribution of the spent fuel composition over the reactor core at the time of the accident.…”

Section: Introductionmentioning

confidence: 99%

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Spatially resolved analysis of plutonium isotopic signatures in environmental particle samples by laser ablation-MC-ICP-MS

Konegger-Kappel

Prohaska

2015

Anal Bioanal Chem

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Laser ablation–multi-collector–inductively coupled plasma mass spectrometry (LA-MC-ICP-MS) was optimized and investigated with respect to its performance for determining spatially resolved Pu isotopic signatures within radioactive fuel particle clusters. Fuel particles had been emitted from the Chernobyl nuclear power plant (ChNPP) where the 1986 accident occurred and were deposited in the surrounding soil, where weathering processes caused their transformation into radioactive clusters, so-called micro-samples. The size of the investigated micro-samples, which showed surface alpha activities below 40 mBq, ranged from about 200 to 1000 μm. Direct single static point ablations allowed to identify variations of Pu isotopic signatures not only between distinct fuel particle clusters but also within individual clusters. The resolution was limited to 100 to 120 μm as a result of the applied laser ablation spot sizes and the resolving power of the nuclear track radiography methodology that was applied for particle pre-selection. The determined 242Pu/239Pu and 240Pu/239Pu isotope ratios showed a variation from low to high Pu isotope ratios, ranging from 0.007(2) to 0.047(8) for 242Pu/239Pu and from 0.183(13) to 0.577(40) for 240Pu/239Pu. In contrast to other studies, the applied methodology allowed for the first time to display the Pu isotopic distribution in the Chernobyl fallout, which reflects the differences in the spent fuel composition over the reactor core. The measured Pu isotopic signatures are in good agreement with the expected Pu isotopic composition distribution that is typical for a RBMK-1000 reactor, indicating that the analyzed samples are originating from the ill-fated Chernobyl reactor. The average Pu isotope ratios [240Pu/239Pu = 0.388(86), 242Pu/239Pu = 0.028(11)] that were calculated from all investigated samples (n = 48) correspond well to previously published results of Pu analyses in contaminated samples from the vicinity of the Chernobyl NPP [e.g. 240Pu/239Pu = 0.394(2) and 242Pu/239Pu = 0.027(1); Nunnemann et al. (J Alloys Compd 271–273:45–48, 1998)].Graphical AbstractEvaluation of LA-MC-ICP-MS for spatially resolving ultra-trace Pu isotopic signatures stored in environmental radioactive particles, providing new insights into the Pu isotopic distribution of the Chernobyl reactor core at the time of the accident

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Spatially resolved analysis of plutonium isotopic signatures in environmental particle samples by laser ablation-MC-ICP-MS

Konegger-Kappel

Prohaska

2015

Anal Bioanal Chem

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“…It was demonstrated the ability of RIMS to detect plutonium in hot -i.e. highly radioactive -aerosol particles and to measure the Pu isotopic composition [84]. After thermal vaporization, 239 Pu atoms were specifically ionized by a triple-resonance ionization scheme [53].…”

Section: Off-line Methodologies Used To Analyze Inorganic Compoundsmentioning

confidence: 99%

Potential of laser mass spectrometry for the analysis of environmental dust particles—A review

Aubriet¹,

Carré²

2010

Analytica Chimica Acta

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“…The advantages of α-spectrometry are relatively low costs of devices needed and high availability in the institutes performing radionuclide analyses. Compared to α-spectrometry lower detection limits and higher isotopic resolution can be achieved by more sophisticated methods RIMS (Resonance Ionisation Mass Spectrometry) [6,7] and ICP-MS [8,9]. With these methods also the isotope ratio 239 Pu/ 240 Pu can be determined which gives important additional information especially when sources of environmental plutonium contamination are evaluated.…”

Section: Introductionmentioning

confidence: 99%

Method for determining plutonium in air filters in detection of nuclear activities

Salminen¹,

Outola²,

Jaakkola³

et al. 2004

Radiochimica Acta

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Plutonium / Air filters / Isotope ratios / Safeguard / Extraction chromatography / SemipalatinskSummary. A method was developed to determine activities and isotope ratios of plutonium and uranium. The method includes dry and wet ashing of air filters and separation of plutonium and uranium from each other and from other nuclides on Eichrom  's extraction chromatography resins UTEVA and TRU. Interferences in plutonium separation caused by thorium and polonium were investigated and eliminated.A field trial was performed in Kurchatov, Kazakhstan, to test the aerosol sampling and radiochemical methods developed for plutonium and uranium. In the air samples collected, the activity of 239,240 Pu varied between 0.67 and 228 Bq/kg of dust, the activity of 238 Pu from 0.20 Bq/kg to 16.4 Bq/kg of dust, and the isotopic ratio 238 Pu/ 239,240 Pu between 0.011 and 2.4. Concentrations of Pu isotopes in the air were 13.4-2490 nBq/m 3 for 239,240 Pu and 7.2-960 nBq/m 3 for 238 Pu. Radioactivity of 239,240 Pu in air filters from Astana varied between 0.075 and 0.72 Bq per kg of dust and that of 238 Pu between 0.038 and 0.14 Bq/kg of dust. Activity concentration of 239,240 Pu in the air of Astana was 5.0-130 nBq/m 3 .

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Determination of isotopic composition of plutonium in hot particles of the Chernobyl area

Cited by 47 publications

References 4 publications

Spatially resolved analysis of plutonium isotopic signatures in environmental particle samples by laser ablation-MC-ICP-MS

Spatially resolved analysis of plutonium isotopic signatures in environmental particle samples by laser ablation-MC-ICP-MS

Potential of laser mass spectrometry for the analysis of environmental dust particles—A review

Method for determining plutonium in air filters in detection of nuclear activities

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