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Authors: Schönenbach, Daniela
Berg, Felix
Breckheimer, Markus
Hagenlocher, Daniel
Schönberg, Pascal
Haas, Raphael
Amayri, Samer
Reich, Tobias
Title: Development, characterization, and first application of a resonant laser secondary neutral mass spectrometry setup for the research of plutonium in the context of long-term nuclear waste storage
Online publication date: 27-Jun-2022
Language: english
Abstract: Plutonium is a major contributor to the radiotoxicity in a long-term nuclear waste repository; therefore, many studies have focused on interactions of plutonium with the technical, geotechnical, and geological barriers of a possible nuclear waste storage site. In order to gain new insights into the sorption on surfaces and diffusion of actinides through these complex heterogeneous materials, a highly sensitive method with spatial resolution is required. Resonant laser secondary neutral mass spectrometry (Laser-SNMS) uses the spatial resolution available in time-of-flight secondary ion mass spectrometry (TOF-SIMS) in combination with the high selectivity, sensitivity, and low background noise of resonance ionization mass spectrometry (RIMS) and is, therefore, a promising method for the study and analysis of the geochemical behavior of plutonium in long-term nuclear waste storage. The authors present an approach with a combined setup consisting of a commercial TOF-SIMS instrument and a Ti:sapphire (Ti:Sa) laser system, as well as its optimization, characterization, and improvements compared to the original proof of concept by Erdmann et al. (2009). As a first application, the spatial distributions of plutonium and other elements on the surface of a pyrite particle and a cement thin section were measured by Laser-SNMS and TOF-SIMS, respectively. These results exemplify the potential of these techniques for the surface analysis of heterogeneous materials in the context of nuclear safety research.
DDC: 540 Chemie
540 Chemistry and allied sciences
Institution: Johannes Gutenberg-Universität Mainz
Department: FB 09 Chemie, Pharmazie u. Geowissensch.
Place: Mainz
Version: Published version
Publication type: Zeitschriftenaufsatz
License: CC BY
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Journal: Analytical and bioanalytical chemistry
Pages or article number: 3987
Publisher: Springer
Publisher place: Berlin u.a.
Issue date: 2021
ISSN: 1618-2650
Publisher DOI: 10.1007/s00216-021-03350-3
Appears in collections:JGU-Publikationen

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