Sensitive redox speciation of iron, neptunium, and plutonium by capillary electrophoresis hyphenated to inductively coupled plasma sector field mass spectrometry

Analytical Chemistry
Carl-Heinrich GraserHorst Geckeis

Abstract

The long-term safety assessment for nuclear waste repositories requires a detailed understanding of actinide (geo)chemistry. Advanced analytical tools are required to gain insight into actinide speciation in a given system. The geochemical conditions in the vicinity of a nuclear repository control the redox state of radionuclides, which in turn has a strong impact on their mobility. Besides the long-lived radionuclides plutonium (Pu) and neptunium (Np), which are key elements in high level nuclear waste, iron (Fe) represents a main component in natural systems controlling redox-related geochemical processes. Measuring the oxidation state distribution for redox sensitive radionuclides and other metal ions is challenging at trace concentrations below the detection limit of most available spectroscopic methods (≥10(-6) M). Consequently, ultrasensitive new analytical techniques are required. Capillary electrophoresis (CE) is a suitable separation method for metal cations. CE hyphenated to inductively coupled plasma sector field mass spectrometry (CE-ICP-SF-MS) was used to measure the redox speciation of Pu (III, IV, V, VI), Np (IV, V, VI), and Fe (II, III) at concentrations lower than 10(-7) M. CE coupling and separation parameters...Continue Reading

References

Aug 13, 2002·Analytical and Bioanalytical Chemistry·Yoshihiro Saito, Kiyokatsu Jinno
Oct 12, 2012·Analytical and Bioanalytical Chemistry·Nils StöbenerTobias Reich
Feb 2, 2013·Chemical Reviews·Marcus AltmaierThomas Fanghänel
Apr 23, 2013·Applied Radiation and Isotopes : Including Data, Instrumentation and Methods for Use in Agriculture, Industry and Medicine·S H LeeJ Sakalys
Dec 25, 2013·Journal of Contaminant Hydrology·Harald Zänker, Christoph Hennig

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Citations

Jan 24, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Sandrine Sauge-MerleJean Aupiais
Oct 27, 2016·Electrophoresis·Anna TýčováKarel Klepárník

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