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Lookup NU author(s): Dr Anna Isakova, Dr Billy Murdoch, Professor Katarina Novakovic
This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License (CC BY-NC-ND).
Palladium-catalysed oxidative carbonylation (PCOC) of alkynes is a promising engine for building smart pulsatile polymeric systems, as it has demonstrated (in certain configurations) sustained regular oscillations in pH and redox potential for up to one month of monitoring in a batch reactor. Recent developments in polymer-supported palladium catalysts allowed to demonstrate the full capacity of this reaction - in a macrogel that experienced oscillations in volume, while releasing a drug load. In this work, we demonstrate reproducible oscillations (more than 100 h duration) in proline-functionalised chitosan-palladium system (Chi-Pro-Pd), using both small molecule (phenylacetylene) and polymeric (pegylated dialkyne) substrate, for the first time. Moreover, by functionalising chitosan with proline ligands, we dramatically reduced halide-mediated leaching of palladium, which readily occurred in non-functionalised chitosan-palladium catalysts (Chi-Pd). Oscillatory patterns for both systems confirm the need for fabricating functionalised chitosan supports to improve catalyst reusability and minimise loss of palladium.
Author(s): Isakova A, Parkes GE, Murdoch BJ, Topham PD, Novakovic K
Publication type: Article
Publication status: Published
Journal: European Polymer Journal
Year: 2018
Volume: 109
Pages: 537-543
Print publication date: 01/12/2018
Online publication date: 25/10/2018
Acceptance date: 24/10/2018
Date deposited: 17/12/2018
ISSN (print): 0014-3057
ISSN (electronic): 1873-1945
Publisher: Elsevier
URL: https://doi.org/10.1016/j.eurpolymj.2018.10.038
DOI: 10.1016/j.eurpolymj.2018.10.038
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