Collaboration between Trinuclear Aluminum Complexes Bearing Bipyrazoles in the Ring-Opening Polymerization of ϵ-Caprolactone

Someswara Rao Kosuru, Feng Jie Lai, Yu Lun Chang, Chen Yu Li, Yi Chun Lai, Shangwu Ding, Kuo Hui Wu, Hsuan Ying Chen, Yung Han Lo

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Abstract

Trinuclear aluminum complexes bearing bipyrazoles were synthesized, and their catalytic activity for ϵ-caprolactone (CL) polymerization was investigated. DBu2Al3Me5 exhibited higher catalytic activity than did the dinuclear aluminum complex LBu2Al2Me4 (16 times as high for CL polymerization; [CL]:[DBu2Al3Me5]:[BnOH] = 100:0.5:5, [DBu2Al3Me5] = 10 mM, conversion 93% after 18 min at room temperature). Density functional theory calculations revealed a polymerization mechanism in which CL first approached the central Al atom and then moved to an external Al. The coordinated CL ring was opened because the repulsion of two tert-butyl groups on the ligands pushed an alkoxide initiator on an external Al to initiate CL. In these trinuclear Al catalysts, the central Al plays a role in monomer capture and then collaborates with the external Al to activate CL, accelerating polymerization.

Original languageEnglish
Pages (from-to)10535-10549
Number of pages15
JournalInorganic Chemistry
Volume60
Issue number14
DOIs
StatePublished - 19 Jul 2021

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