Multi-element isotopic analysis of hot particles from Chornobyl

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Autoren

  • Darcy van Eerten
  • Manuel Alexander Christoph Raiwa
  • Paul Hanemann
  • Laura Leifermann
  • Tobias Weissenborn
  • Wolfgang Dietrich Schulz
  • Martin Weiß
  • Danielle Ziva Shulaker
  • Peter Boone
  • David Willingham
  • Keenan Thomas
  • Brian Sammis
  • Brett Isselhardt
  • Mike Savina
  • Clemens Walther

Externe Organisationen

  • Lawrence Livermore National Laboratory
Forschungs-netzwerk anzeigen

Details

OriginalspracheEnglisch
Aufsatznummer131338
FachzeitschriftJournal of hazardous materials
Jahrgang452
Frühes Online-Datum1 Apr. 2023
PublikationsstatusVeröffentlicht - 15 Juni 2023

Abstract

Microscopic fuel fragments, so-called “hot particles”, were released during the 1986 accident at the Chornobyl
nuclear powerplant and continue to contaminate the exclusion zone in northern Ukraine. Isotopic analysis can
provide vital information about sample origin, history and contamination of the environment, though it has been
underutilized due to the destructive nature of most mass spectrometric techniques, and inability to remove
isobaric interference. Recent developments have diversified the range of elements that can be investigated
through resonance ionization mass spectrometry (RIMS), notably in the fission products. The purpose of this
study is to demonstrate the application of multi-element analysis on hot particles as relates to their burnup,
particle formation in the accident, and weathering. The particles were analysed with two RIMS instruments:
resonant-laser secondary neutral mass spectrometry (rL-SNMS) at the Institute for Radiation Protection and
Radioecology (IRS) in Hannover, Germany, and laser ionization of neutrals (LION) at Lawrence Livermore Na-
tional Laboratory (LLNL) in Livermore, USA. Comparable results across instruments show a range of burnup
dependent isotope ratios for U and Pu and Cs, characteristic of RBMK-type reactors. Results for Rb, Ba and Sr
show the influence of the environment, retention of Cs in the particles and time passed since fuel discharge.

Schlagwörter

    RIMS, Actinides, Fission products, Ultra-trace analysis

ASJC Scopus Sachgebiete

Zitieren

Multi-element isotopic analysis of hot particles from Chornobyl. / van Eerten, Darcy; Raiwa, Manuel Alexander Christoph; Hanemann, Paul et al.
in: Journal of hazardous materials, Jahrgang 452, 131338, 15.06.2023.

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

van Eerten, D, Raiwa, MAC, Hanemann, P, Leifermann, L, Weissenborn, T, Schulz, WD, Weiß, M, Ziva Shulaker, D, Boone, P, Willingham, D, Thomas, K, Sammis, B, Isselhardt, B, Savina, M & Walther, C 2023, 'Multi-element isotopic analysis of hot particles from Chornobyl', Journal of hazardous materials, Jg. 452, 131338. https://doi.org/10.1016/j.jhazmat.2023.131338
van Eerten, D., Raiwa, M. A. C., Hanemann, P., Leifermann, L., Weissenborn, T., Schulz, W. D., Weiß, M., Ziva Shulaker, D., Boone, P., Willingham, D., Thomas, K., Sammis, B., Isselhardt, B., Savina, M., & Walther, C. (2023). Multi-element isotopic analysis of hot particles from Chornobyl. Journal of hazardous materials, 452, Artikel 131338. https://doi.org/10.1016/j.jhazmat.2023.131338
van Eerten D, Raiwa MAC, Hanemann P, Leifermann L, Weissenborn T, Schulz WD et al. Multi-element isotopic analysis of hot particles from Chornobyl. Journal of hazardous materials. 2023 Jun 15;452:131338. Epub 2023 Apr 1. doi: 10.1016/j.jhazmat.2023.131338
van Eerten, Darcy ; Raiwa, Manuel Alexander Christoph ; Hanemann, Paul et al. / Multi-element isotopic analysis of hot particles from Chornobyl. in: Journal of hazardous materials. 2023 ; Jahrgang 452.
Download
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title = "Multi-element isotopic analysis of hot particles from Chornobyl",
abstract = "Microscopic fuel fragments, so-called “hot particles”, were released during the 1986 accident at the Chornobylnuclear powerplant and continue to contaminate the exclusion zone in northern Ukraine. Isotopic analysis canprovide vital information about sample origin, history and contamination of the environment, though it has beenunderutilized due to the destructive nature of most mass spectrometric techniques, and inability to removeisobaric interference. Recent developments have diversified the range of elements that can be investigatedthrough resonance ionization mass spectrometry (RIMS), notably in the fission products. The purpose of thisstudy is to demonstrate the application of multi-element analysis on hot particles as relates to their burnup,particle formation in the accident, and weathering. The particles were analysed with two RIMS instruments:resonant-laser secondary neutral mass spectrometry (rL-SNMS) at the Institute for Radiation Protection andRadioecology (IRS) in Hannover, Germany, and laser ionization of neutrals (LION) at Lawrence Livermore Na-tional Laboratory (LLNL) in Livermore, USA. Comparable results across instruments show a range of burnupdependent isotope ratios for U and Pu and Cs, characteristic of RBMK-type reactors. Results for Rb, Ba and Srshow the influence of the environment, retention of Cs in the particles and time passed since fuel discharge.",
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T1 - Multi-element isotopic analysis of hot particles from Chornobyl

AU - van Eerten, Darcy

AU - Raiwa, Manuel Alexander Christoph

AU - Hanemann, Paul

AU - Leifermann, Laura

AU - Weissenborn, Tobias

AU - Schulz, Wolfgang Dietrich

AU - Weiß, Martin

AU - Ziva Shulaker, Danielle

AU - Boone, Peter

AU - Willingham, David

AU - Thomas, Keenan

AU - Sammis, Brian

AU - Isselhardt, Brett

AU - Savina, Mike

AU - Walther, Clemens

N1 - This Marie Sklodowska-Curie Action (MSCA) Innovative Training Network (ITN) receives funding from the European Union’s H2020 Framework Programme under grant agreement no. 861198. Parts of this work was performed under the auspices of the U.S. Department of En- ergy by Lawrence Livermore National Laboratory, and was partially supported by the National Nuclear Security Agency Office of Defense Nuclear Nonproliferation Research and Development. LLNL-JRNL- 844531. Additional thanks goes to Klaus Wendt and his group at Johannes Gutenberg University in Mainz for laser development and continued advice.

PY - 2023/6/15

Y1 - 2023/6/15

N2 - Microscopic fuel fragments, so-called “hot particles”, were released during the 1986 accident at the Chornobylnuclear powerplant and continue to contaminate the exclusion zone in northern Ukraine. Isotopic analysis canprovide vital information about sample origin, history and contamination of the environment, though it has beenunderutilized due to the destructive nature of most mass spectrometric techniques, and inability to removeisobaric interference. Recent developments have diversified the range of elements that can be investigatedthrough resonance ionization mass spectrometry (RIMS), notably in the fission products. The purpose of thisstudy is to demonstrate the application of multi-element analysis on hot particles as relates to their burnup,particle formation in the accident, and weathering. The particles were analysed with two RIMS instruments:resonant-laser secondary neutral mass spectrometry (rL-SNMS) at the Institute for Radiation Protection andRadioecology (IRS) in Hannover, Germany, and laser ionization of neutrals (LION) at Lawrence Livermore Na-tional Laboratory (LLNL) in Livermore, USA. Comparable results across instruments show a range of burnupdependent isotope ratios for U and Pu and Cs, characteristic of RBMK-type reactors. Results for Rb, Ba and Srshow the influence of the environment, retention of Cs in the particles and time passed since fuel discharge.

AB - Microscopic fuel fragments, so-called “hot particles”, were released during the 1986 accident at the Chornobylnuclear powerplant and continue to contaminate the exclusion zone in northern Ukraine. Isotopic analysis canprovide vital information about sample origin, history and contamination of the environment, though it has beenunderutilized due to the destructive nature of most mass spectrometric techniques, and inability to removeisobaric interference. Recent developments have diversified the range of elements that can be investigatedthrough resonance ionization mass spectrometry (RIMS), notably in the fission products. The purpose of thisstudy is to demonstrate the application of multi-element analysis on hot particles as relates to their burnup,particle formation in the accident, and weathering. The particles were analysed with two RIMS instruments:resonant-laser secondary neutral mass spectrometry (rL-SNMS) at the Institute for Radiation Protection andRadioecology (IRS) in Hannover, Germany, and laser ionization of neutrals (LION) at Lawrence Livermore Na-tional Laboratory (LLNL) in Livermore, USA. Comparable results across instruments show a range of burnupdependent isotope ratios for U and Pu and Cs, characteristic of RBMK-type reactors. Results for Rb, Ba and Srshow the influence of the environment, retention of Cs in the particles and time passed since fuel discharge.

KW - RIMS

KW - Actinides

KW - Fission products

KW - Ultra-trace analysis

KW - Actinides

KW - Fission products

KW - RIMS

KW - Ultra-trace analysis

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JO - Journal of hazardous materials

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M1 - 131338

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