Journal
DALTON TRANSACTIONS
Volume 43, Issue 28, Pages 10739-10750Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c4dt00863d
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- Natural Sciences and Engineering Research Council (NSERC) of Canada
- Canada Foundation for Innovation (CFI)
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The pyrrole-based ligand N,N'-((1H-pyrrole-2,5-diyl)bis(diphenylphosphoranylylidene))bis(4- isopropyl-aniline) (HLB) can be deprotonated and coordinated to yttrium and samarium ions upon reaction with their respective trialkyl precursors. In the case of yttrium, the resulting complex [LBY(CH2SiMe3)(2)] (1) is a Lewis base-free monomer that is remarkably resistant to cyclometalation. Conversely, the analogous samarium complex [LBSm(CH2SiMe3)(2)] is dramatically more reactive and undergoes rapid orthometalation of one phosphinimine aryl substituent, generating an unusual 4-membered azasamaracyclic THF adduct [kappa(4)-LBSm(CH2SiMe3)(THF)(2)] (2). This species undergoes further transformation in solution to generate a new dinuclear species that features unique carbon and nitrogen bridging units [kappa(1):kappa(2):mu(2)-LBSm(THF)](2) (3). Alternatively, if 2 is intercepted by a second equivalent of HLB, the doubly-ligated samarium complex [(kappa(4)-L-B)LBSm] (4) forms.
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