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Procedures for precise measurements of 135Cs/137Cs atom ratios in environmental samples at extreme dynamic ranges and ultra-trace levels by thermal ionization mass spectrometry

Research output: Contribution to journalArticle

Original languageEnglish
Pages (from-to)347-356
Number of pages10
JournalTalanta
Volume174
Early online date13 Jun 2017
DOIs
DateAccepted/In press - 12 Jun 2017
DateE-pub ahead of print - 13 Jun 2017
DatePublished (current) - 1 Nov 2017

Abstract

Determination of 135Cs/137Cs atom ratios has the potential to be a powerful tool for nuclear forensics and monitoring environmental processes. We present optimized chemical separation techniques and thermal ionization mass spectrometry (TIMS) protocols to obtain precise 135Cs/137Cs atom ratios for a range of environmental sample types. We use a combination of double AMP-PAN separation and Sr-spec resin column purification to yield excellent separation from the alkali metals (Rb separation factor > 600), which normally suppress ionization of Cs. A range of emission activators for the ionization of Cs were evaluated and glucose solution yielded the optimal combination of a stable Cs+ beam, minimal low-temperature polyatomic interferences and improved ionization efficiency. Mass-spectrometric determination of low abundance 135Cs and 137Cs is compromised by the presence of a very large 133Cs+ beam, which may be scattered and cause significant spectral interferences. These are explored using multi-static Faraday cup – ion counter methods and a range of energy filter settings. The method is evaluated using environmental samples and standards from regions affected by fallout from Chernobyl (IAEA-330) and Fukushima nuclear disasters. Where the intensity of 133Cs+ is large relative to 135Cs+ and 137Cs+ (< 30 cps), minor polyatomic interferences need to be considered. In the absence of a standard with 135, 137Cs/133Cs < 1 × 10−8, we explored the reproducibility of 135Cs/137Cs atom ratios at these high dynamic ranges and extremely low abundance (137Cs ≈ 12 fg g−1) for sediments from an estuarine setting in SW England, UK.

    Research areas

  • Radiocaesium, TIMS, Interferences, Scattered 133Cs+

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    Rights statement: This is the final published version of the article (version of record). It first appeared online via Elsevier at https://doi.org/10.1016/j.talanta.2017.06.033 . Please refer to any applicable terms of use of the publisher.

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