Simple Zn(ii) complexes for the production and degradation of polyesters

Jack Stewart; Martin  Fuchs; Jack Payne; Oli Driscoll; Gabrielle Kociok-Kohn; Benjamin Ward; Sonja Herres-Pawlis; Matthew Jones

doi:10.1039/D1RA09087A

Simple Zn(ii) complexes for the production and degradation of polyesters

Jack Stewart
, Martin Fuchs
, Jack Payne
, Oli Driscoll
, Gabrielle Kociok-Kohn
, Benjamin Ward
, Sonja Herres-Pawlis
, Matthew Jones

RWTH Aachen University
Cardiff University
Technische Universität Dortmund

Research output: Contribution to journal › Article › peer-review

39 Citations (SciVal)

Abstract

Nine new complexes based on thioether appended iminophenolate (ONS) ligands have been prepared and fully characterized in solution by NMR spectroscopy. Solid-state structures were also obtained for seven complexes. In solution, all complexes were monomeric. The complexes were highly active for the polymerization of purified rac-lactide ([M] : [Zn] : [BnOH] = 10 000 : 1 : 30 at 180 °C) reaching TOF values up to 250 000 h−1. The kinetics of the polymerization have been probed by in situ Raman spectroscopy. The rate of reaction was dramatically reduced using technical grade rac-lactide with increased initiator loading. To move towards a circular economy, it is vital that catalysts are developed to facilitate chemical recycling of commodity and emerging polymeric materials. In this vein, the complexes have been assessed for their ability to break down poly(lactic acid) and poly(ethylene terephthalate). The results from both the polymerization and degradation reactions are discussed in terms of ligand functionality.

Original language	English
Pages (from-to)	1416-1424
Number of pages	9
Journal	RSC Advances
Volume	12
Issue number	3
Early online date	7 Jan 2022
DOIs	https://doi.org/10.1039/D1RA09087A
Publication status	Published - 7 Jan 2022

Bibliographical note

Funding Information:
We would like to thank the EPSRC for funding a PhD studentship to JS (EP/L016443/1) and for funding for JP (EP/L016354/1). The University of Bath (OD) and MC2 are acknowledged for their use of facilities. We thank the EPSRC National Crystallographic Service center for collection of data for Zn(2)2. This study was partly funded under the Excellence Strategy of the Federal Government and the Länder (G: (DE-82)EXS-PF-KA007).

Publisher Copyright:
© 2022 The Royal Society of Chemistry.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 8 Decent Work and Economic Growth
SDG 12 Responsible Consumption and Production

ASJC Scopus subject areas

General Chemistry
General Chemical Engineering

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10.1039/D1RA09087ALicence: CC BY

Cite this

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abstract = "Nine new complexes based on thioether appended iminophenolate (ONS) ligands have been prepared and fully characterized in solution by NMR spectroscopy. Solid-state structures were also obtained for seven complexes. In solution, all complexes were monomeric. The complexes were highly active for the polymerization of purified rac-lactide ([M] : [Zn] : [BnOH] = 10 000 : 1 : 30 at 180 °C) reaching TOF values up to 250 000 h−1. The kinetics of the polymerization have been probed by in situ Raman spectroscopy. The rate of reaction was dramatically reduced using technical grade rac-lactide with increased initiator loading. To move towards a circular economy, it is vital that catalysts are developed to facilitate chemical recycling of commodity and emerging polymeric materials. In this vein, the complexes have been assessed for their ability to break down poly(lactic acid) and poly(ethylene terephthalate). The results from both the polymerization and degradation reactions are discussed in terms of ligand functionality.",

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AU - Ward, Benjamin

AU - Herres-Pawlis, Sonja

AU - Jones, Matthew

N1 - Funding Information: We would like to thank the EPSRC for funding a PhD studentship to JS (EP/L016443/1) and for funding for JP (EP/L016354/1). The University of Bath (OD) and MC2 are acknowledged for their use of facilities. We thank the EPSRC National Crystallographic Service center for collection of data for Zn(2)2. This study was partly funded under the Excellence Strategy of the Federal Government and the Länder (G: (DE-82)EXS-PF-KA007). Publisher Copyright: © 2022 The Royal Society of Chemistry.

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N2 - Nine new complexes based on thioether appended iminophenolate (ONS) ligands have been prepared and fully characterized in solution by NMR spectroscopy. Solid-state structures were also obtained for seven complexes. In solution, all complexes were monomeric. The complexes were highly active for the polymerization of purified rac-lactide ([M] : [Zn] : [BnOH] = 10 000 : 1 : 30 at 180 °C) reaching TOF values up to 250 000 h−1. The kinetics of the polymerization have been probed by in situ Raman spectroscopy. The rate of reaction was dramatically reduced using technical grade rac-lactide with increased initiator loading. To move towards a circular economy, it is vital that catalysts are developed to facilitate chemical recycling of commodity and emerging polymeric materials. In this vein, the complexes have been assessed for their ability to break down poly(lactic acid) and poly(ethylene terephthalate). The results from both the polymerization and degradation reactions are discussed in terms of ligand functionality.

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Simple Zn(ii) complexes for the production and degradation of polyesters

Abstract

Bibliographical note

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ASJC Scopus subject areas

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