Kinetics of the Wet Oxidation of Phenol over an Fe/Activated Carbon Catalyst
Kinetics of the Wet Oxidation of Phenol over an Fe/Activated Carbon Catalyst
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DOI：
10.2202/1542-6580.1555
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发表时间：
2007-12
影响因子：
1.6
通讯作者：
A. Quintanilla;J. Casas;J. J. Rodríguez-J.;M. Kreutzer;F. Kapteijn;J. Moulijn
中科院分区：
文献类型：
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作者：
A. Quintanilla;J. Casas;J. J. Rodríguez-J.;M. Kreutzer;F. Kapteijn;J. Moulijn
在滴流床反应器中研究了Fe/活性炭催化剂上苯酚的湿式氧化反应，操作条件为：入口C苯酚=0.5和1 g/L，T=100-127 °C，PT=3-8 atm，W=0-4.8 g，QL=0.125-2 mL/min，QO_2 =91.6 NmL/min。苯酚的氧化和矿化反应是通过非均相机理在催化剂表面进行的。由于苯酚氧化路线的复杂性，简单的反应方案已假定通过集中的中间物种和广义动力学模型苯酚和TOC减排已被提出。两个动力学表达式，幂律速率和朗缪尔-欣谢尔伍德型速率表达式，已被认为是，但只有收敛与统计上可靠的参数被发现前一个模型。苯酚氧化反应的动力学模型为一级动力学模型，氧的动力学模型为0.74，表观活化能为74 kJ/mol。苯酚的矿化（TOC减排）描述了一个类似的速率表达式，并考虑到存在的难熔物质，如苯酚氧化后形成的低分子量酸。
Wet oxidation of phenol over an Fe/activated carbon catalyst has been studied in a trickle-bed reactor in the following operational window: inlet C phenol=0.5 and 1 g/L, T=100-127 °C, PT=3-8 atm, W=0-4.8 g, QL=0.125-2 mL/min and QO2=91.6 NmL/min. The experiments were carried out in the absence of mass transfer limitations. Oxidation and mineralization reactions of phenol are proven to take place on the catalyst surface through a heterogeneous mechanism. Due to the complexity of the phenol oxidation route, simple reaction schemes have been assumed by lumping the intermediate species and generalized kinetic models for phenol and TOC abatement have been proposed. Two kinetic expressions, a power law rate and a Langmuir-Hinshelwood type rate expression, have been considered but only a convergence with statistically reliable parameters was found for the former model. A power law model with first order for phenol and 0.74 for oxygen and apparent activation energy of 74 kJ/mol described the experimental results in the oxidation of phenol well. Mineralization of phenol (TOC abatement) was described by a similar rate expression and takes into account the presence of refractory species such as the low molecular weight acids formed upon phenol oxidation.