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Lookup NU author(s): Dr James Leach, Professor Katarina NovakovicORCiD
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Oscillatory palladium-catalysed oxidative carbonylation reactions, named the BT-GN reactions after their core contributors Bruk, Temkin, Gorodsky and Novakovic, have garnered attention due to their ability to under batch-like conditions produce long lasting (minutes to weeks) oscillations in pH, redox potential, turbidity, and heat of the reaction. [1] This makes the BT-GN reactions an attractive prospect for use as a driving force in smart materials, such as pH responsive hydrogels. The BT-GN reactions take place under lab conditions where complex products are formed from simple starting materials. In many of the studies phenylacetylene is used as a substrate and palladium iodide as a catalyst. [2] To use them in polymeric smart materials such as a hydrogels the BT GN reaction must be adapted to produce oscillations in pH within a polymeric framework, therefore the substrate and catalyst must be replaced with polymeric analogues. In our recent studies we shown that other palladium catalysts and a polymeric alkyne-based substrate PEGA (poly(ethylene glycol) methyl ether acetylene) can produced oscillations in pH. Furthermore a proof-of-concept study demonstrated a self oscillating chitosan macrogel with phenylacetylene as a substrate. [3], [4] This talk will cover advances in the BT-GN reaction with reactions between the polymeric catalyst, chitosan-2-pyridylimine palladium chloride (Chi-IM-PdCl2) and polymer substrate (PEGA) in both solution and hydrogels. References [1] K. Novakovic, L. Bruk, and O. Temkin, “History, versatility and future prospects of oscillatory carbonylation reactions of alkynes.,” RSC Adv., vol. 11, no. 39, pp. 24336–24344, Jul. 2021, doi: 10.1039/d1ra03810a. [2] O. N. Temkin and L. G. Bruk, “Palladium(II, I, 0) Complexes in Catalytic Reactions of Oxidative Carbonylation,” Kinet. Catal., vol. 44, no. 5, pp. 601–617, 2003, doi: 10.1023/A:1026161103700. [3] L. Donlon and K. Novakovic, “Oscillatory carbonylation using alkyne-functionalised poly(ethylene glycol),” Chem. Commun., vol. 50, no. 98, pp. 15506–15508, 2014, doi: 10.1039/c4cc01548g. [4] A. Isakova and K. Novakovic, “Pulsatile release from a flat self-oscillating chitosan macrogel,” J. Mater. Chem. B, vol. 6, no. 30, pp. 5003–5010, 2018, doi: 10.1039/c8tb00781k.
Author(s): Leach J, Novakovic K
Publication type: Conference Proceedings (inc. Abstract)
Publication status: Published
Conference Name: ACS Meeting Spring 2024
Year of Conference: 2024
Print publication date: 17/03/2024
Online publication date: 17/03/2024
Acceptance date: 04/12/2023
Publisher: ACS
URL: https://www.acs.org/meetings/acs-meetings.html
