期刊
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
卷 413, 期 15, 页码 3987-3997出版社
SPRINGER HEIDELBERG
DOI: 10.1007/s00216-021-03350-3
关键词
Plutonium; Laser-SNMS; Resonant laser ionization; Ultra-trace analysis; TOF-SIMS; Nuclear waste
资金
- FederalMinistry of Education and Research (BMBF) [02NUK044B]
The study focuses on the interaction of plutonium with barriers at nuclear waste storage sites and introduces a highly sensitive method combining TOF-SIMS and RIMS for analyzing plutonium's geochemical behavior in long-term nuclear waste storage.
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.
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