Multiactinide Analysis with Accelerator Mass Spectrometry for Ultratrace Determination in Small Samples: Application to an in Situ Radionuclide Tracer Test within the Colloid Formation and Migration Experiment at the Grimsel Test Site (Switzerland)

Autor(en)

Francesca Quinto, Ingo Blechschmidt, Carmen Garcia Perez, Horst Geckeis, Frank Geyer, Robin Golser, Florian Huber, Markus Lagos, Bill Lanyon, Markus Plaschke, Peter Steier, Thorsten Schaefer

Abstrakt

The multiactinide analysis with accelerator mass spectrometry (AMS) was applied to samples collected from the run 13-05 of the Colloid Formation and Migration (CFM) experiment at the Grimsel Test Site (GTS). In this in situ radionuclide tracer test, the environmental behavior of U-233, Np-237, Pu-242, and Am-243 was investigated in a water conductive shear zone under conditions relevant for a nuclear waste repository in crystalline rock. The concentration of the actinides in the GTS groundwater was determined with AMS over 6 orders of magnitude from similar to 15 pg/g down to similar to 25 ag/g. Levels above 10 fg/g were investigated with both sector field inductively coupled plasma mass spectrometry (SF-ICPMS) and AMS. Agreement within a relative uncertainty of 50% was found for Np-237, Pu-242, and Am-243 concentrations determined with the two analytical methods. With the extreme sensitivity of AMS, the long-term release and retention of the actinides was investigated over 8 months in the tailing of the breakthrough curve of run 13-05 as well as in samples collected up to 22 months after. Furthermore, the evidence of masses 241 and 244 u in the CFM samples most probably representing Am-241 and Pu-244 employed in a previous tracer test demonstrated the analytical capability of AMS for in situ studies lasting more than a decade.

Organisation(en)

Isotopenphysik

Externe Organisation(en)

Karlsruher Institut für Technologie, Nationale Genossenschaft für die Lagerung radioaktiver Abfälle, Rheinische Friedrich-Wilhelms-Universität Bonn, Fracture Systems Ltd, Friedrich-Schiller-Universität Jena

Journal

Analytical Chemistry

Band

89

Seiten

7182-7189

Anzahl der Seiten

8

ISSN

0003-2700

DOI

https://doi.org/10.1021/acs.analchem.7b01359

Publikationsdatum

07-2017

Peer-reviewed

Ja

ÖFOS 2012

103014 Kernphysik, 104002 Analytische Chemie

Schlagwörter

Link zum Portal

https://ucris.univie.ac.at/portal/de/publications/multiactinide-analysis-with-accelerator-mass-spectrometry-for-ultratrace-determination-in-small-samples-application-to-an-in-situ-radionuclide-tracer-test-within-the-colloid-formation-and-migration-experiment-at-the-grimsel-test-site-switzerland(9202dcf7-7e06-49e4-a0de-d2ac70a8e396).html