A series of aluminium iminophosphoranylenamide complexes, [Me2Al{N(Ar)C(Ph)CHP(Ph2)N-Ar1}] (Ar = Ph, Ar1 = p-MeC6H4 (9); Ar = Ph, Ar1 = o-ClC6H4 (10); Ar = Ph, Ar1 = o-FC6H4 (11); Ar = p-MeC6H4, Ar1 = o-FC6H4 (12)), were synthesised by the reactions of ArNC(Ph)CH2P(Ph2)NAr1 (5–8) with AlMe3 in toluene. Similar reactions between o-{ArNP(Ph2)}C6H4NHC(Ph)CHP(Ph2)NAr (Ar = p-MeC6H4, 13), and AlMe3 in toluene generates aluminium iminophosphoranylanilide, 14. All new compounds were characterised by NMR spectroscopy and elemental analysis. The molecular structures of complexes 9 and 14 were further characterised by single-crystal X-ray structure determination. In the presence of benzyl alcohol (BnOH) each of the complexes is catalytically active for the ring-opening polymerisation (ROP) of ε-caprolactone (ε-CL), and complex 14 has the highest activity among them.
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