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Uranium(iv) terminal hydrosulfido and sulfido complexes: insights into the nature of the uranium-sulfur bond.


ABSTRACT: Herein, we report the synthesis and characterization of a series of terminal uranium(iv) hydrosulfido and sulfido complexes, supported by the hexadentate, tacn-based ligand framework (Ad,MeArO)3tacn3- (= trianion of 1,4,7-tris(3-(1-adamantyl)-5-methyl-2-hydroxybenzyl)-1,4,7-triazacyclononane). The hydrosulfido complex [((Ad,MeArO)3tacn)U-SH] (2) is obtained from the reaction of H2S with the uranium(iii) starting material [((Ad,MeArO)3tacn)U] (1) in THF. Subsequent deprotonation with potassium bis(trimethylsilyl)amide yields the mononuclear uranium(iv) sulfido species in good yields. With the aid of dibenzo-18-crown-6 and 2.2.2-cryptand, it was possible to isolate a terminal sulfido species, capped by the potassium counter ion, and a "free" terminal sulfido species with a well separated cation/anion pair. Spectroscopic and computational analyses provided insights into the nature of the uranium-sulfur bond in these complexes.

SUBMITTER: Rosenzweig MW 

PROVIDER: S-EPMC6024247 | BioStudies | 2016-01-01

REPOSITORIES: biostudies

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