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Autonomous reorganisation of the oscillatory phase in the PdI2 catalysed phenylacetylene carbonylation reaction

Lookup NU author(s): Dr Julie Parker, Dr Katarina Novakovic

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


Abstract

The PdI2 catalysed oxidative carbonylation of phenylacetylene has been shown to produce pH oscillations over the temperature range 0-40 °C under semi-batch conditions. The decrease in reaction temperature resulted in an increase in the period and amplitude of the pH oscillations. In addition, reducing the reaction temperature enabled the observation of different phases in the oscillatory pH behaviour confirming the ability of the reaction system to autonomously produce multiple clusters of oscillatory phases. Sets of pH oscillations were recorded at 0 and 10 °C. At temperatures of 0-20 °C oscillations commenced as pH was falling during the initial stages of the reaction while, at 30 and 40 °C, the oscillations commenced once the pH started to increase after the initial drop. Oscillations in turbidity were observed at 20 and 30 °C. Experiments were conducted in an HEL Simular reaction calorimeter enabling precise temperature control. Operating at 0 °C reduced the reaction rate prolonging the duration of pH oscillations. The oscillatory pH behaviour was recorded for 11 days without additional substrate at which point the run was terminated although the oscillations would likely have continued.


Publication metadata

Author(s): Parker J, Novakovic K

Publication type: Article

Publication status: Published

Journal: Reaction Kinetics, Mechanisms and Catalysis

Year: 2016

Pages: 1-13

Online publication date: 11/02/2016

Acceptance date: 15/01/2016

Date deposited: 09/03/2016

ISSN (print): 1878-5190

ISSN (electronic): 1878-5204

Publisher: Springer

URL: http://dx.doi.org/10.1007/s11144-016-0979-8

DOI: 10.1007/s11144-016-0979-8


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