Single-Site Calcium Initiators for the Controlled Ring-Opening Polymerization of Lactides and Lactones

SummarySingle-site calcium initiators containing chelating tmhd (H-tmhd = 2,2,6,6-tetramethylheptane-33-dione) ligands [(THF)Ca(tmhd)]2[μ-N(SiMe3)2](μ-tmhd) (2) and [(THF)Ca(tmhd)]2[μ-OCH(Me)Ph](μ-tmhd) (3) have been synthesized and applied for the ring-opening polymerization of L-lactide and ε-caprolactone. Both 2 and 3 were highly reactive and promoted a fast polymerization of L-lactide and ε-caprolactone to high monomer conversions under mild conditions (THF as a solvent, room temperature). More importantly, results showed that the ring-opening polymerizations of lactides and lactones initiated by either 3 or 2 in the presence of equivalent 2-propanol are living, to provide polymers and block copolymers of controlled molecular weights and tailored end-groups. The polymerizations were first-order in monomer up to high conversions, in which the in situ initiating system 2/2-propanol revealed no induction period and much faster polymerization kinetics as compared to 3.