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Free imine imidazol-2-imine ligands with two different substitution patterns have been isolated for the first time and they were found to exist as an equilibrium mixture of geometric and mesomeric isomers. The relative ratios of these isomers are dependent on both the nature of the substituents and of the solvent. The synthesis of the titanium(IV) alkyl and arylimido complexes of these ligands was unexpectedly found to be very selective and was successfully achieved only with the lesser sterically-demanding 2,4,6-trimethylphenyl derivative IMesN^Imine 2a. The solid-state structure of the alkylimido complex further confirms the zwitterionic character of the ligand. The isolated titanium imido complexes were found to be active catalysts for the polymerisation of ethylene.
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