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

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 [UO 2(NO 3) 2(TBP) 2], [UO 2(NO 3) 2(H 2O)(TBP) 2], and [UO 2(NO 3) 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 [UO 2(DBP)], [UO 2(DBP) 3], and [UO 2(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.
Authors:
 [1] ;  [2] ;  [3] ;  [4]
  1. Univ. of Utah, Salt Lake City, UT (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  3. Commissariat a l'Energie Atomique et aux Energies Alternatives (CEA-Saclay), Gif-sur-Yvette (France)
  4. Washington State Univ., Pullman, WA (United States)
Publication Date:
Report Number(s):
PNNL-SA-116620
Journal ID: ISSN 0003-2700
Grant/Contract Number:
SC0004102; HDTRA11010111; AC05-76RL01830; NA0000582
Type:
Published Article
Journal Name:
Analytical Chemistry
Additional Journal Information:
Journal Volume: 88; Journal Issue: 5; Journal ID: ISSN 0003-2700
Publisher:
American Chemical Society (ACS)
Research Org:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1237779
Alternate Identifier(s):
OSTI ID: 1249357