Abstract
The reactivity of the uranium tuck-in and tuck-over cyclopentadienyl moieties {[η5:η1-C5Me4CH2]U}2+ and {U[μ-η5:η1-C5Me4CH2]U}6+, respectively, has been investigated by examining the reactivity of (C5Me5)U[μ-η5:η1:η1-C5Me3(CH2)2](μ-H)2U(C5Me5)2, 1, and (C5Me5)(η5:η1-C5Me4CH2)(hpp)U [(hpp)− = 1,3,4,6,7,8-hexahydro-2H-pyrimido[1,2-a]pyrimidinato], 2, with hydrogen, silyl halide, sulfide, amine, and hydrocarbon reagents. The reactivity of 2, which has a single tuck-in reactive site, provides valuable comparisons with that of 1, where the presence of two hydride ligands as well as both tuck-in and tuck-over moieties leads to products in which multiple transformations have occurred. Both 1 and 2 react with H2 to form hydrides, namely, the [(C5Me5)2UH2]2/[(C5Me5)2UH]2 equilibrium mixture and (C5Me5)2(hpp)UH, 3, respectively. Attempts to make a simple chloride derivative of 1 with Me3SiCl yielded a new tethered metallocene, (C5Me5)ClU(η5-C5Me4CH2SiMe2CH2-κC), 4, which formally results from a silylmethyl C−H bond...
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