Carvalho R H, Lemos F, Lemos M A N D A, Vojinović V, Fonseca L P, Cabral J M S
Centro de Engenharia Biológica e Química, Departmento Engenharia Química, Instituto Superior Técnico, Av. Rovisco Pais, 1049-001, Lisbon, Portugal.
Bioprocess Biosyst Eng. 2006 Jul;29(2):99-108. doi: 10.1007/s00449-006-0057-0. Epub 2006 Apr 13.
Phenol is an industrial pollutant and its removal from industrial wastewaters is of great importance. In order to design optimised phenol removal procedures by using horseradish peroxidase-based systems, there are some points that have to be dealt with. One of the most important issues is the need for reliable kinetics as this is one of the difficulties found during process scale-up. Although simplified kinetics can be used for limited ranges of operating conditions, they are not usually reliable for the description of varying process conditions. The present work describes the implementation of a kinetic model, based on a mechanism, for the co-oxidation of phenol and 4-aminoantipyrine (Am-NH2), which is used as a chromogen agent, with hydrogen peroxide as the oxidant. The model covers not only the variation of the concentrations of all the species involved, but also the effect of temperature in the reaction. The estimation of kinetic rate constants and activation energies for the various steps in the mechanism is performed with a single optimisation procedure, and all the experimental results are described using a unique set of parameters, which, thus, is valid over an extended range of operating conditions. The mechanism allowed the determination of a reliable kinetic model which is appropriate for the range of experimental conditions used. The computational model was also tested with an independent set of experiments with different conditions from the ones for which the parameters were estimated.
苯酚是一种工业污染物，从工业废水中去除苯酚至关重要。为了设计基于辣根过氧化物酶体系的优化苯酚去除程序，有一些要点必须加以处理。最重要的问题之一是需要可靠的动力学，因为这是工艺放大过程中遇到的困难之一。虽然简化的动力学可用于有限的操作条件范围，但它们通常不可靠，无法描述变化的工艺条件。本工作描述了基于一种机理的动力学模型的实施，该模型用于苯酚与用作显色剂的4-氨基安替比林（Am-NH2）以过氧化氢为氧化剂的共氧化反应。该模型不仅涵盖了所有相关物种浓度的变化，还包括温度对反应的影响。通过单一优化程序对机理中各个步骤的动力学速率常数和活化能进行估计，并且所有实验结果都使用一组唯一的参数进行描述，因此该参数在扩展的操作条件范围内有效。该机理使得能够确定一个适用于所用实验条件范围的可靠动力学模型。该计算模型还通过一组独立实验进行了测试，这些实验的条件与估计参数时所用的条件不同。
