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We here report the synthesis and characterization of a complete series of terminal hydrochalcogenido, U-EH, and chalcogenido uranium(iv) complexes, U≡E (with E = O, S, Se, Te), supported by the ( Ad,Me ArOH) 3 acn (1,4,7-tris(3-(1-adamantyl)-5-methyl-2-hydroxybenzyl)-1,4,7-triazacyclononane) ligand system. Reaction of H 2 E with the trivalent precursor [(( Ad,Me ArO) 3 acn)U] (1) yields the corresponding uranium(iv) hydrochalcogenido complexes [(( Ad,Me ArO) 3 acn)U(EH)] (2). Subsequent deprotonation of the terminal hydrochalcogenido species with KN(SiMe 3 ) 2 , in the presence of 2.2.2-cryptand, gives access to the uranium(iv) complexes with terminal chalcogenido ligands [K(2.2.2-crypt)][(( Ad,Me ArO) 3 acn)U≡E] (3). In order to study the influence of the varying terminal chalogenido ligands on the overall molecular and electronic structure, all complexes were studied by single-crystal X-ray diffractometry, UV/vis/NIR, electronic absorption, and IR vibrational spectroscopy as well as SQUID magnetometry and computational analyses (DFT, MO, NBO).

A complete series of uranium(iv) complexes with terminal hydrochalcogenido (EH) and chalcogenido (E) ligands E = O, S, Se, Te