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A novel symmetric pyrazine (pyz)-bridged uranyl dimer [UOCl(HO)(Pyz)]: synthesis, structure and computational analysis. | LitMetric
Herein we report on the synthesis of (HPyz)[UOCl(HO)(Pyz)]·2HO which features a novel pyrazine-bridged uranyl dimer, [UOCl(HO)(Pyz)]. A rigorous computational and experimental analysis of this compound was performed to fully explore the influence of coordination on the electronic structure and potential charge-transfer characteristics of this dimer, revealing a delocalized π-system across the bridging pyrazine and the axial components of both uranyl centers. Electrostatic surface potentials, used to rationalize the observed assembly, indicate a decreased basicity of the uranyl oxo [UOCl], and signify a lessened capacity for the terminal -yl oxos of the [UOCl(HO)(Pyz)] dimer to participate in supramolecular assembly. A combined density functional theory (DFT) and quantum theory of atoms in molecules (QTAIM) analysis further evidenced an increase in UO bond strengths within the dimer, which is supported by a blue shift in the characteristic Raman-active uranyl symmetric stretch () with respect to the more typically observed [UOCl].
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