Details
| Translated title of the contribution | Multielement-Ultraspurennachweis von Radionukliden in Umweltproben |
|---|---|
| Original language | English |
| Qualification | Doctor rerum naturalium |
| Awarding Institution | |
| Supervised by |
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| Thesis sponsors |
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| Date of Award | 21 May 2024 |
| Place of Publication | Hannover |
| Publication status | Published - 11 Jun 2024 |
Abstract
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Hannover, 2024. 130 p.
Research output: Thesis › Doctoral thesis
}
TY - BOOK
T1 - Multi-element ultra-trace detection of radionuclides in environmental samples
AU - van Eerten, Darcy
PY - 2024/6/11
Y1 - 2024/6/11
N2 - A ‘hot particle’ is a microscopic fragment deriving from nuclear material. The detection of these particles is in some cases the first marker of the release of nuclear material. Its history is contained in its isotopic composition, characteristic of its origin and interaction with the environment. This work focuses on environmental samples derived from the accident sites in Chornobyl and Fukushima, studied through resonant ionisation mass spectrometry, RIMS. The principle of RIMS relies on the universality of atomic structure to selectively analyse isotope ratios in a target element. This work discusses the design and operation of different instruments. Individual hot particles were analysed in the SIRIUS RIMS instrument at the Institute for Radiation Protection and Radioecology (IRS) in Hannover, Germany. A comparison study was done on eight Chornobyl Exclusion Zone (CEZ) particles with the LION at Lawrence Livermore National 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. Isotopic analysis therefore provides vital information about sample origin and degradation. In most mass spectrometric techniques without laser ionisation, the removal of isobaric interference requires chemical pre-treatment, thereby destroying the sample. This limits their application for isotopic analysis, necessitating a focus on one or two elements only, as allowed by small sample size. The versatility offered by multi-element RIMS makes it uniquely suited to the study of individual hot particles. In this work, isotope ratio analysis has been expanded to the actinides U, Pu, Np, and Am, and the fission products Rb, Sr, Zr, Cs and Ba. Isotope ratio analysis is interpreted in the contexts of nuclear forensics, radioecology, and reactor physics. A collection of samples can be grouped by analysing the time-dependent Sr, show how flux changes the U, Pu, and Cs composition across a reactor, and show through Ba that Cs has been lost to the environment.
AB - A ‘hot particle’ is a microscopic fragment deriving from nuclear material. The detection of these particles is in some cases the first marker of the release of nuclear material. Its history is contained in its isotopic composition, characteristic of its origin and interaction with the environment. This work focuses on environmental samples derived from the accident sites in Chornobyl and Fukushima, studied through resonant ionisation mass spectrometry, RIMS. The principle of RIMS relies on the universality of atomic structure to selectively analyse isotope ratios in a target element. This work discusses the design and operation of different instruments. Individual hot particles were analysed in the SIRIUS RIMS instrument at the Institute for Radiation Protection and Radioecology (IRS) in Hannover, Germany. A comparison study was done on eight Chornobyl Exclusion Zone (CEZ) particles with the LION at Lawrence Livermore National 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. Isotopic analysis therefore provides vital information about sample origin and degradation. In most mass spectrometric techniques without laser ionisation, the removal of isobaric interference requires chemical pre-treatment, thereby destroying the sample. This limits their application for isotopic analysis, necessitating a focus on one or two elements only, as allowed by small sample size. The versatility offered by multi-element RIMS makes it uniquely suited to the study of individual hot particles. In this work, isotope ratio analysis has been expanded to the actinides U, Pu, Np, and Am, and the fission products Rb, Sr, Zr, Cs and Ba. Isotope ratio analysis is interpreted in the contexts of nuclear forensics, radioecology, and reactor physics. A collection of samples can be grouped by analysing the time-dependent Sr, show how flux changes the U, Pu, and Cs composition across a reactor, and show through Ba that Cs has been lost to the environment.
U2 - 10.15488/17441
DO - 10.15488/17441
M3 - Doctoral thesis
CY - Hannover
ER -