Determination of Lanthanides, Thorium, Uranium and Plutonium in Irradiated (Th, Pu)O2 by Liquid Chromatography Using α-Hydroxyiso Butyric Acid (α-HIBA)

Pranaw Kumar, P. G. Jaison, Vijay M. Telmore, Sumana Paul, Suresh K. Aggarwal

Fuel Chemistry Division, Bhabha Atomic Research Centre, Mumbai, India.

DOI: 10.4236/ijamsc.2013.11009                

Abstract

An HPLC method is presented for the separation and determination of lanthanides (Lns), thorium (Th), uranium (U) and plutonium (Pu) from irradiated (Th, Pu)O₂. Individual separation of Lns, Th, U and Pu is a challenging task becauseof 1) lanthanideshavingsimilar physical and chemical properties, 2) presence of complex matrix like irradiated fuel and 3) the co-existence of multiple oxidation states of Pu. Different procedures were developed for separation of individual lanthanides and actinides.The individual lanthanides were separated on a dynamically modified reversed phase (RP) column using n-octane sulfonic acid as an ion interaction reagentand employingdual gradient(pH and concentration) of α-hydroxyisobutyric acid (HIBA). In order to improve the precision on the determination of Lns, terbium (Tb) was used as an internal standard. The method was validated employing simulated high level liquid waste. Concentrations of lanthanides viz. lanthanum (La) and neodymium (Nd) in the dissolver solution were determined based on their peak areas. Th, U and Pu were separated on a RP column using mobile phase containing HIBA and methanol. Since Pu is prone to exist in multiple oxidation states, all the oxidation states were converted into Pu (IV) using H₂O₂ in 3M HNO₃. Under the optimized conditions, Pu(IV) eluted first followed by Th and U. The concentrations of Th, U and Pu were determined by standard addition method andwere found to be 1.10 ± 0.02 mg/g, 5.3 ± 0.3 μg/g and 27 ± 1 μg/g, respectively, in the dissolver solution of irradiated fuel. These values were in good agreement with the concentration of Th determined by biamperometry and those of U and Puby isotope dilution thermal ionization mass spectrometry.

Keywords

HPLC; Lanthanides; Th; U; Pu; ?-HIBA; Irradiated (Th, Pu)O2

Conflicts of Interest

The authors declare no conflicts of interest.

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