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Eur. J. Mass Spectrom. 4, 47 - 54 (1998)

Identification of isomeric tributylphosphate dimers formed by radiolysis using tandem mass spectrometry and stable isotopic labelling

Denis Lesage,* Henri Virelizier and Christopher K. Jankowski
DCC/DPE/SPEA/SAIS, Centre détudes Nucléaires de Saclay, 91191 Gif-sur-Yvette, France.
Jean Claude Tabet
Laboratoire de Chimie Structurale Organique et Biologique, EP103, Université P. et M. Curie, 4 place Jussieu, 75252 Paris Cedex 05, France.

ABSTRACT:
Tributylphosphate (TBP) dimers, formed during radiolysis of the nuclear fuel reprocessing solvent, were studied using tandem mass spectrometry (MS/MS), stable isotopic labelling (2H) and synthetic model compounds. The structures of isomeric dimers and their lower homologues were established, using GC/MS as well as electron impact and chemical ionisation GC/tandem mass spectrometry, with an extensive use of ion chromatograms of characteristic fragment ions from collision-induced decomposition in both non-deuterated and selectively deuterated series. An explanation of isomer ratios and of the restricted number of lower homologues as well as a radiolytic mechanism are advanced. The TBP-dimer fraction represented less than ~ 0.03% of the total mixture obtained from radiolysis of solvent.

Keywords: Tributylphosphate, tributylphosphate dimers, radiolysis, tandem mass spectrometry, phosphate, PUREX.

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