Abstract
A general strategy for the determination of Tc oxidation state by new approach involving X-ray absorption near edge spectroscopy (XANES) at the Tc L3 edge is shown. A comprehensive series of 99Tc compounds, ranging from oxidation states I to VII, was measured and subsequently simulated within the framework of crystal-field multiplet theory. The observable trends in the absorption edge energy shift in combination with the spectral shape allow for a deeper understanding of complicated Tc coordination chemistry. This approach can be extended to numerous studies of Tc systems as this method is one of the most sensitive methods for accurate Tc oxidation state and ligand characterization.
Highlights
A first general strategy for the determination of Technetium oxidation state by a new approach involving X-ray absorption near edge spectroscopy (XANES) at the Tc L3 edge is shown for series of 99Tc compounds, ranging from oxidation states I to VII
A well-defined oxidation state in coordination species is of paramount importance, since ligand atoms can be connected differently to the coordination center, depending on its oxidation state
Electronic supplementary information (ESI)†) can provide complementary information about ligands and their coordination, but lack sensitivity when compared to Tc L3 edge XANES
Summary
A comprehensive series of 99Tc compounds, ranging from oxidation states I to VII, was measured and subsequently simulated within the framework of crystal-field multiplet theory. Note that an even larger reduction of the Slater integral values has been suggested[31] for 4d transition element solids versus molecular systems in these type of calculations to take into account the effect of the Tc 4d hybridization with ligand states.
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