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Broadening the scope of Pd-catalysed oscillatory carbonylation reactions: solvent, substrate, catalyst

Lookup NU author(s): Dr Anna Isakova, Dr Julie Parker, Chinyelumndy Nwosu, Professor Katarina Novakovic

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This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0).


Abstract

On our way to producing all-polymeric self-oscillatory materials, we have expanded the horizons of oscillatory carbonylation reactions by searching for alternative substrates, solvents and even catalysts. In this paper, we demonstrate that pH oscillations in carbonylation reactions have the potential to occur in a broad range of aliphatic alcohol solutions when using either a small molecule substrate (phenylacetylene) or a polymeric substrate (pegylated alkyne) with either a small molecule catalyst (Pd-diacetate) or a non-leaching polymeric catalyst (Pd-polyacrylate). The alcohols studied are methanol, ethanol, 1-propanol, 1-butanol and 1-hexanol. In this carbonylation reaction an alcohol serves as both the solvent and as a reactant. The resulting oscillations suggest that carbonylation reactions have strong potential for the discovery and development of new oscillatory chemical systems. Replacing methanol, commonly used in oscillatory carbonylation processes, with ethanol is an important step in enhancing the biocompatibility of these systems. Furthermore, showing that oscillations in pH are feasible in ethanol solutions when polymeric substrate and polymeric catalyst are used supports the vision of employing oscillatory chemical reactions to build oscillatory materials.


Publication metadata

Author(s): Isakova A, Parker J, Nwosu CJ, Howse JR, Novakovic K

Publication type: Article

Publication status: Published

Journal: Reaction Kinetics, Mechanisms and Catalysis

Year: 2019

Volume: 127

Issue: 1

Pages: 161-174

Print publication date: 01/06/2019

Online publication date: 09/03/2019

Acceptance date: 04/03/2019

Date deposited: 04/03/2019

ISSN (print): 1878-5190

ISSN (electronic): 1878-5204

Publisher: Akademiai Kiado Rt.

URL: https://doi.org/10.1007/s11144-019-01563-3

DOI: 10.1007/s11144-019-01563-3

Data Access Statement: https://doi.org/10.17634/153345-3

Notes: Ref.: Ms. No. REAC-D-18-00631R1


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Funding

Funder referenceFunder name
EP/N033655/1EPSRC

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