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

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  Publication Details (including relevant citation   information):

  Novakovic, K.; Grosjean, C.; Scott, S. K.; Whiting, A.; Willis,   M. J.; Wright, A. R. Chem. Phys. Lett.,   2007, 435, 142‐147


  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.

  Address (URL): 24739&_coverDate=02%2F12%2F2007&_alid=1743128999&_rdoc=1&_fmt=high&_orig=search & _origin=search&_zone=rslt_list_item&_cdi=5231&_sort=r&_st=13&_docanchor=&view=c & _ct=1&_acct=C000014659&_version=1&_urlVersion=0&_userid=224739&md5=9a5362a30bca 7 596c5e2b8ff52d3d72f&searchtype=a