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Title: Failure of ESI Spectra to Represent Metal-Complex Solution Composition: A Study of Lanthanide-Carboxylate Complexes

Electrospray ionization - mass spectrometry (ESI-MS) was used for the characterization of uranyl complexed to tributyl phosphate (TBP) and dibutyl phosphate (DBP). The stoichiometry of uranyl with TBP and DBP was determined, and the gas phase speciation was found to be dependent on the cone voltage applied to induce fragmentation on the gas phase complexes. To quantitatively compare the gas phase distribution of species to solution, apparent stability constants were calculated. With a cone voltage of 80V, the apparent stability constants for the complexes UO2(NO3)2•2TBP, UO2(NO3)2(H2O)•2TBP, and UO2(DBP)+ were determined. With a lower cone voltage applied, larger complexes were observed and stability constants for the complexes UO2(NO3)2•3TBP and UO2(DBP)42- were determined.
Authors:
; ;
Publication Date:
OSTI Identifier:
1225169
Report Number(s):
PNNL-SA-96226
Journal ID: ISSN 0003-2700; WN0219080
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Analytical Chemistry; Journal Volume: 86; Journal Issue: 2
Publisher:
American Chemical Society (ACS)
Research Org:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
Uranium, Solvent Extraction, PUREX, Actinides, Complexation, Nuclear Reprocessing, Electrospray Ionization