Abstract
The placement of a strongly trans-influencing ligand on a ruthenium center opposite an anchoring silyl group of the tetradentate tripodal tris(phosphino)silyl ligand, [SiPPh3]− ([SiPPh3]− = tris(2-(diphenylphosphino)phenyl)silyl), has been explored. Installation of alkyl or terminal phosphide ligands trans to the anchoring silyl group affords the complexes [SiPPh3]RuR (R = Me (2), CH2Ph (4), PPh2 (5), PiPr2 (6)). Complexes 2, 4, and 5 are thermally unstable. Complexes 2 and 4 decay to the cyclometalated complex [SiPPh2P′Ph]Ru (3), whereas complex 5 decays to the cyclometalated phosphine adduct [SiPPh2P′Ph]Ru(PHPh2) (7). Complex 3 is found to effect E−H (E = H, C, Si, Ge) bond activation of substrates such as secondary silanes and germanes to yield the structurally unusual silylene complexes [SiPPh3]Ru(H)(SiRR′) (R = R′ = Ph (10a), R = Ph R′ = Me (10b)) and the germylene complex [SiPPh3]Ru(H)(GeR2) (R = Ph) (11) via double E−H activation transformations. Both theory and experiments suggest electrophilic ch...
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