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Combining alkali metals and zinc to harness heterometallic cooperativity in cyclic ester ring-opening polymerisation

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Abstract

Heterometallic cooperativity is an emerging strategy to elevate polymerisation catalyst performance. Here, we report the first heterotrimetallic Na/Zn2 and K/Zn2 complexes supported by a ProPhenol ligand, which deliver “best of both” in cyclic ester ring-opening polymerisation, combining the outstanding activity (Na/K) and good control (Zn2) of homometallic analogues. Detailed NMR studies and density-functional theory calculations suggest that the Na/Zn2 and K/Zn2 complexes retain their heterometallic structures in the solution-state. To the best of our knowledge, the K/Zn2 analogue is the most active heterometallic catalyst reported for rac-lactide polymerisation (kobs = 1.7 × 10−2 s−1), giving activities five times faster than the Na/Zn2 complex. These versatile catalysts also display outstanding performance in ε-caprolatone and δ-valerolactone ring-opening polymerisation. These studies provide underpinning methodologies for future heterometallic polymerisation catalyst design, both in cyclic ester polymerisation and other ring-opening (co)polymerisation reactions.

Graphical abstract: Combining alkali metals and zinc to harness heterometallic cooperativity in cyclic ester ring-opening polymerisation

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Supplementary files

Article information


Submitted
26 Aug 2020
Accepted
05 Oct 2020
First published
12 Oct 2020

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2020, Advance Article
Article type
Edge Article

Combining alkali metals and zinc to harness heterometallic cooperativity in cyclic ester ring-opening polymerisation

W. Gruszka, A. Lykkeberg, G. S. Nichol, M. P. Shaver, A. Buchard and J. A. Garden, Chem. Sci., 2020, Advance Article , DOI: 10.1039/D0SC04705H

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