On the use of time resolved laser induced fluorescence and nano electrospray ionization mass spectrometry for radionuclides sulfate speciation

ANYL 83

Christophe Moulin, christophe.moulin@cea.fr, Thomas Vercouter, Pierre Vitorge, and Badia Amekraz, badia.amekraz@cea.fr. Department of Nuclear Energy, CEA, DPC/SECR/LSRM, Bat 391, 91191 Gif sur yvette, France
Predicting speciation of radionuclides in natural environment is still of great interest for nuclear waste disposal. In this framework, lanthanides complexation by sulfate (present in natural water) has been investigated by complementary speciation techniques. The formation of La-sulfate complexes was studied by nanoelectrospray ionization mass spectrometry (nanoESI-MS). Several gaseous species containing LaSO4+ were detected. In addition, time-resolved laser-induced fluorescence(TRLIF) was used to study Eu-sulfate speciation under similar conditions. Complexing constant obtained by both methods are in good agreement. This confirms the potential of nanoESIMS for the study of kinetically labile species. La(SO4)2- was also detected and the complexing constant determined. Fluorescence lifetimes measured for Eu-sulfate complexes are consistent with the replacement of one water molecule in the Eu first coordination sphere for each added sulfate ligand, suggesting a monodentate sulfate coordination. Future trends in radionuclides speciation such as uranium, plutonium,... by TRLIF and nanoESI-MS will also be given as well as improvements in nuclearisation of these speciation techniques.
 

General Papers
7:00 PM-9:00 PM, Sunday, 10 September 2006 Moscone Center -- Hall D, Poster

Division of Analytical Chemistry

The 232nd ACS National Meeting, San Francisco, CA, September 10-14, 2006