Combining polymer-bound catalyst with polymeric substrate for reproducible pH oscillations in palladium-catalysed oxidative carbonylation of alkynes

Isakova, A, Parkes, G, Murdoch, B, Topham, P and Novakovic, K 2018, 'Combining polymer-bound catalyst with polymeric substrate for reproducible pH oscillations in palladium-catalysed oxidative carbonylation of alkynes', European Polymer Journal, vol. 109, pp. 537-543.


Document type: Journal Article
Collection: Journal Articles

Title Combining polymer-bound catalyst with polymeric substrate for reproducible pH oscillations in palladium-catalysed oxidative carbonylation of alkynes
Author(s) Isakova, A
Parkes, G
Murdoch, B
Topham, P
Novakovic, K
Year 2018
Journal name European Polymer Journal
Volume number 109
Start page 537
End page 543
Total pages 7
Publisher Pergamon Press
Abstract 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 have demonstrated 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 a 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.
Subject Catalysis and Mechanisms of Reactions
DOI - identifier 10.1016/j.eurpolymj.2018.10.038
Copyright notice © 2018 Elsevier
ISSN 0014-3057
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