Achieving pH and Qr oscillations in a palladium-catalysed phenylacetylene oxidative carbonylation reaction using an automated reactor system
Achieving pH and Qr oscillations in a palladium-catalysed phenylacetylene oxidative carbonylation reaction using an automated reactor system
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DOI：
10.1016/j.cplett.2006.12.040
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发表时间：
2007-02-12
影响因子：
2.8
通讯作者：
Wright, A. R.
中科院分区：
文献类型：
--
作者：
Novakovic, K.;Grosjean, C.;Wright, A. R.
本文报道了在均相催化体系（PdI_2-KI-空气-乙酸钠甲醇溶液）中，钯催化苯乙炔氧化羰基化反应过程中pH值和热输出（Qr）的可重复振荡的实验研究。实验在精确控制温度和气体流速的HEL SIMULAR（TM）反应量热计中进行。在某些实验条件下，观察到第二组振荡。Qr的振荡是放热的，没有相应的吸热。振荡过程中释放的总能量遵循阶梯函数，最大值为600 J/振荡。热释放与pH下降同步，并随pH升高而降低。(c)2006 Elsevier B. V.保留所有权利。
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 (TM) 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. (c) 2006 Elsevier B.V. All rights reserved.