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


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.

Share and Cite:

Bera, S. , Balasubramanian, R. , Datta, A. , Sajimol, R. , Nalini, S. , S. Lakshmi Narasimhan, T. , P. Antony, M. , Sivaraman, N. , Nagarajan, K. and R. Vasudeva Rao, P. (2013) Burn-Up Measurements on Dissolver Solution of Mixed Oxide Fuel Using HPLC-Mass Spectrometric Method. International Journal of Analytical Mass Spectrometry and Chromatography, 1, 55-60. doi: 10.4236/ijamsc.2013.11007.

Conflicts of Interest

The authors declare no conflicts of interest.


[1] J. E. Rein and B. F. Rider, “TID-17385, Burn-Up Determination of Nuclear Fuels,” Progress Report, AEC Research and Development Report, 1962.
[2] ASTM Standards E, “Standard Test Method for Atom Percent Fission in Uranium and Plutonium Fuel (Neodymium-148 Method),” ASTM Standards E321-96, 2005.
[3] C. H. Knight, R. M. Cassidy, B. M. Recoskie and L. W. Green, “Dynamic Ion Exchange Chromatography for Determination of Number of Fissions in Thorium-Uranium Dioxide Fuels,” Analytical Chemistry, Vol. 56, No. 3, 1984, pp. 474-478. doi:10.1021/ac00267a041
[4] R. M. Cassidy, S. Elchuk, N. L. Elliot, L. W. Green, C. H. Knight and B. M. Recoskie, “Dynamic Ion Exchange Chromatography for the Determination of Number of Fissions in Uranium Dioxide Fuels,” Analytical Chemistry, Vol. 58, No. 6, 1986, pp. 1181-1186. doi:10.1021/ac00297a045
[5] N. Sivaraman, S. Subramaniam, T. G. Srinivasan and P. R. Vasudeva Rao, “Burn-Up Measurements on Nuclear Reactor Fuels Using High Performance Liquid Chromatography,” Journal of Radioanalytical and Nuclear Chemistry, Vol. 253, No. 1, 2002, pp. 35-40. doi:10.1023/A:1015800114488
[6] R. Balasubramanian, D. Darwin Albert Raj, S. Nalini and M. Sai Baba, “Mass Spectrometric Studies on Irradiated (U, Pu) Mixed Carbide Fuel of FBTR,” International Journal of Nuclear Energy Science and Technology, Vol. 1, No. 2-3, 2005, pp. 197-203.
[7] A. Datta, N. Sivaraman, T. G. Srinivasan and P. R. Vasudeva Rao, “Single Stage Dual Column HPLC Technique for Separation and Determination of Lanthanides in Uranium Matrix-Application to Burn-Up Measurement on Nuclear Reactor Fuel,” Nuclear Technology, Vol. 182, 2013, pp. 84-97.
[8] P. G. Jaison, N. M. Raut and S. K. Aggarwal, “Direct Determination of Lanthanides in Simulated Irradiated Thoria Fuels Using Reversed-Phase High-Performance Liquid Chromatography,” Journal of Chromatography A, Vol. 1122, No. 1-2, 2006, pp. 47-53. doi:10.1016/j.chroma.2006.04.037
[9] P. R. Vasudeva Rao, N. Sivaraman and T. G. Srinivasan, “Studies of Lanthanide Separation with HPLC,” In: Encyclopedia of Chromatography, Taylor & Francis, 2005.
[10] A. Datta, N. Sivaraman, T. G. Srinivasan and P. R. Vasudeva Rao, “Rapid Separation of Lanthanides and Actinides on Small Particle Based Reverse Phase Supports,” Radiochimica Acta, Vol. 98, 2010, pp. 277-285. doi:10.1524/ract.2010.1715
[11] A. Datta, N. Sivaraman, T. G. Srinivasan and P. R. Vasudeva Rao, “Liquid Chromatographic Behaviour of Lanthanide and Actinides on Monolith Supports,” Radiochimica Acta, Vol. 99, 2011, pp. 275-283. doi:10.1524/ract.2011.1816
[12] E. A. C. Crouch, “Atomic Data and Nuclear Data Tables: Fission Product Yields from Neutron Induced Fission,” Academic Press, New York and London, Vol. 19, 1977.

Copyright © 2023 by authors and Scientific Research Publishing Inc.

Creative Commons License

This work and the related PDF file are licensed under a Creative Commons Attribution 4.0 International License.