Burn-Up Measurements on Dissolver Solution of Mixed Oxide Fuel Using HPLC-Mass Spectrometric Method

S. Bera, R. Balasubramanian, Arpita Datta, R. Sajimol, S. Nalini, T. S. Lakshmi Narasimhan, M. P. Antony, N. Sivaraman, K. Nagarajan, P. R. Vasudeva Rao

Chemistry Group, Indira Gandhi Centre for Atomic Research, Kalpakkam, India.

DOI: 10.4236/ijamsc.2013.11007                

Abstract

Burn-up measurement on an irradiated mixed oxide (MOX) test fuel pellet was carried out through measurements on the dissolver solution by HPLC-Thermal Ionization Mass Spectrometric (TIMS) technique. The studies carried out using HPLC as well as TIMS for quantification of burn-up value are described. While in one case, both the separation and determination of elements of interest (U, Pu and Nd) were carried out by HPLC; in another case, TIMS technique was used to quantify them from the HPLC separated fractions.The rapid separation procedures developed in our laboratory earlier were employed to isolate pure fractions of the desired elements. The individual lanthanide fission products (La to Eu) were separated from each other using dynamic ion-exchange chromatographic technique whereas uranium and plutonium were separated from each other using reversed phase chromatographic technique. The pure fractions of U, Pu and Nd obtained after HPLC separation procedure for “spiked” and “unspiked” dissolver solutions were used in TIMS measurements for the first time in our laboratory. In TIMS analysis, isotopic abundances of uranium, plutonium and neodymium fractions obtained from HPLC separation procedure on an “unspiked” fuel sample were measured. For the determination of U, Pu and Nd by isotopic dilution mass spectrometric technique (IDMS), known quantities of tracers enriched in ²³⁸U, ²⁴⁰Pu and ¹⁴²Nd were added to the pre-weighed dissolver solution and subjected to HPLC separation procedures. The isotope ratios viz. ¹⁴²Nd/(¹⁴⁵Nd +¹⁴⁶Nd), ²³⁸U/²³³U and ²⁴⁰Pu/²³⁹Pu in the pertinent “spiked” fractions were subsequently measured by TIMS. The spikes were pre-standardized in our laboratory employing reverse isotopic dilution technique against the standard solutions available in our laboratory (for ²³⁸U, ²³⁹Pu and ¹⁴²Nd, standard solutions of ²³³U, ²³⁹Pu (of higher abundance than in the sample) and ¹⁵⁰Nd were employed as spikes). The burn-up values from duplicate spiking experiments were computed based on the summation of ¹⁴⁵Nd + ¹⁴⁶Nd. The concentrations of neodymium, uranium and plutonium were also measured using HPLC with post-column derivatisation technique using aresenazo(III) as the post-column reagent. The atom % burn-up computed from HPLC and TIMS techniques were in good agreement.

Keywords

MOX; Dissolver Solution; HPLC; TIMS; Uranium; Plutonium; Neodymium

Conflicts of Interest

The authors declare no conflicts of interest.

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