A series of EP(V)-imine phosphine–imine ligands (Dipp-NC(CH3)–(CH2)–PE(Ph2)) (Dipp = 2,6-diisopropylphenyl, E = O, S, Se) and corresponding dimethyl aluminum and indium complexes were prepared and characterized using multi-nuclear NMR spectroscopy and SC-XRD. Solution-state 1H and 31P NMR spectroscopy indicate a mixture of isomers in solution (C6D6, CDCl3, and CD3CN). Solid state structures of both the imine and (E)-enamine isomers of the oxygen-based ligand have been observed. These three ligands (L) were then deprotonated with M(CH3)3 (M = Al or In), with methane loss forming a 6-membered ring via bidentate chelation ((κ2-L)M(CH3)2). The indium/oxide complex also crystallized as a 12-membered ring.
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