Characterization of Actinides Complexed to Nuclear Fuel Constituents Using ESI-MS

Analytical Chemistry
Luther W McDonaldSue B Clark

Abstract

Electrospray ionization-mass spectrometry (ESI-MS) was tested for its use in monitoring spent nuclear fuel (SNF) constituents including U, Pu, dibutyl phosphate (DBP), and tributyl phosphate (TBP). Both positive and negative ion modes were used to evaluate the speciation of U and Pu with TBP and DBP. Furthermore, apparent stability constants were determined for U complexed to TBP and DBP. In positive ion mode, TBP produced a strong signal with and without complexation to U or Pu, but, in negative ion mode, no TBP, U-TBP, or Pu-TBP complexes were observed. Apparent stability constants were determined for [UO2(NO3)2(TBP)2], [UO2(NO3)2(H2O)(TBP)2], and [UO2(NO3)2(TBP)3]. In contrast DBP, U-DBP, and Pu-DBP complexes were observed in both positive and negative ion modes. Apparent stability constants were determined for the species [UO2(DBP)], [UO2(DBP)3], and [UO2(DBP)4]. Analyzing mixtures of U or Pu with TBP and DBP yielded the formation of ternary complexes whose stoichiometry was directly related to the ratio of TBP to DBP. The ESI-MS protocols used in this study will further demonstrate the utility of ESI-MS and its applicability to process control monitoring in SNF reprocessing facilities.

References

Sep 5, 2003·Rapid Communications in Mass Spectrometry : RCM·Valerio B Di MarcoPietro Traldi
Mar 17, 2009·European Journal of Medicinal Chemistry·G-J HeX-G Li
Oct 23, 2010·Physical Chemistry Chemical Physics : PCCP·Xianggui YeBamin Khomami
Sep 29, 2011·Journal of the American Society for Mass Spectrometry·Philip X RutkowskiMichael J Van Stipdonk
Jan 10, 2012·Journal of Mass Spectrometry : JMS·Daniel RiosMichael J Van Stipdonk

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Citations

Apr 13, 2018·Rapid Communications in Mass Spectrometry : RCM·Irena J TatosianMichael J Van Stipdonk
Apr 15, 2018·Journal of the American Society for Mass Spectrometry·Michael J Van StipdonkIrena Tatosian
Jul 4, 2019·Rapid Communications in Mass Spectrometry : RCM·Kaitlin CoopersmithMatthew S Wellons

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