Synthesis of heteroleptic uranium (mu-eta(6):eta(6)-C6H6)2- sandwich complexes via facile displacement of (eta(5)-C5Me5)1- by ligands of lower hapticity and their conversion to heteroleptic bis(imido) compounds

Journal of the American Chemical Society
William J EvansJoseph W Ziller

Abstract

Reactivity studies on the sterically crowded [(C(5)Me(5))(2)U](2)(mu-eta(6):eta(6)-C(6)H(6)), 1, have revealed that eta(1)-ligands can displace one of the normally inert (eta(5)-C(5)Me(5))(1-) ligands in each metallocene unit to form a series of heteroleptic bimetallic sandwich complexes of nonplanar (C(6)H(6))(2-), namely, [(C(5)Me(5))(X)U](2)(mu-eta(6):eta(6)-C(6)H(6)), where X = N(SiMe(3))(2), OC(6)H(2)(CMe(3))(2)-2,6-Me-4, and CH(SiMe(3))(2). Displacement by an amidinate is also possible, that is, X = (i)PrNC(Me)N(i)Pr. This allows the multielectron reactivity of the (mu-eta(6):eta(6)-C(6)H(6))(2-) sandwich complexes to be studied as a function of ancillary ligands. Specifically, the reaction of 1 with K[N(SiMe(3))(2)], previously found to form {(C(5)Me(5))[(Me(3)Si)(2)N]U}(2)(C(6)H(6)), 2, also occurs with K[OC(6)H(2)(CMe(3))(2)-2,6-Me-4], Li[CH(SiMe(3))(2)], and Li[(i)PrNC(Me)N(i)Pr] to form {(C(5)Me(5))[4-Me-2,6-(Me(3)C)(2)C(6)H(2)O]U}(2)(C(6)H(6)), 3, {(C(5)Me(5))[(Me(3)Si)(2)CH]U}(2)(C(6)H(6)), 4, and {(C(5)Me(5))[(i)PrNC(Me)N(i)Pr]U}(2)(C(6)H(6)), 5, respectively. The reactivity of 2-5 vis-a-vis 1 has been compared with the substrates 1,3,5,7-cyclooctatetraene (C(8)H(8)) and 1-azidoadamantane (AdN(3)). Complex 1 acts ...Continue Reading

References

Nov 30, 2004·Chemical Communications : Chem Comm·Shaheed A MungurPolly L Arnold
Sep 22, 2005·Chemical Communications : Chem Comm·William J EvansJoseph W Ziller
Oct 26, 2005·Inorganic Chemistry·William J EvansJoseph W Ziller
Dec 24, 2005·Science·Trevor W HaytonP Jeffrey Hay
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Oct 22, 2008·Chemical Communications : Chem Comm·Liam P SpencerJames M Boncella
Feb 17, 2009·Inorganic Chemistry·Liam P SpencerJames M Boncella
Jun 6, 2009·Angewandte Chemie·Michel Ephritikhine

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Citations

Feb 22, 2012·Inorganic Chemistry·Paula L Diaconescu, Christopher C Cummins
May 5, 2012·Inorganic Chemistry·Stefan G MinasianDavid K Shuh
Nov 26, 2010·Journal of the American Chemical Society·Clément CampMarinella Mazzanti
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Aug 7, 2013·Journal of the American Chemical Society·Clément CampMarinella Mazzanti
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