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Achieving pH and Qr oscillations in a palladium-catalysed phenylacetylene oxidative carbonylation reaction using an automated reactor system

Lookup NU author(s): Professor Katarina Novakovic, Dr Christophe Grosjean, Dr Mark Willis, Professor Allen Wright

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Abstract

This Letter reports an experimental study which achieves reproducible oscillations in both pH and heat output (Qr) during a palladium-catalysed phenylacetylene oxidative carbonylation reaction in an homogeneous catalytic system (PdI2-KI-Air-NaOAc in methanol solution). Experiments were performed in an HEL SIMULAR™ reaction calorimeter with precise control of temperature and gas flow rates. Under certain experimental conditions a second set of oscillations was observed. Oscillations in Qr were exothermic with no corresponding endotherm. Total energy released during oscillations followed a staircase function with a maximum of 600 J/oscillation. Heat release was in phase with pH fall, and decreased as pH increased. © 2006 Elsevier B.V. All rights reserved.

Publication metadata

Author(s): Novakovic K, Grosjean C, Scott SK, Whiting A, Willis MJ, Wright AR

Publication type: Article

Publication status: Published

Journal: Chemical Physics Letters

Year: 2007

Volume: 435

Issue: 1-3

Pages: 142-147

Print publication date: 12/02/2007

ISSN (print): 0009-2614

ISSN (electronic): 1873-4448

Publisher: Elsevier BV

URL: http://dx.doi.org/10.1016/j.cplett.2006.12.040

DOI: 10.1016/j.cplett.2006.12.040

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