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甲苯的催化氧化:粉末状和整体式锰镍混合氧化物催化剂的对比研究

Catalytic oxidation of toluene: comparative study over powder and monolithic manganese-nickel mixed oxide catalysts.

作者信息

Duplančić Marina, Tomašić Vesna, Gomzi Zoran

机构信息

a Department of Reaction Engineering and Catalysis , Faculty of Chemical Engineering and Technology, University of Zagreb , Zagreb , Croatia.

出版信息

Environ Technol. 2018 Aug;39(15):2004-2016. doi: 10.1080/09593330.2017.1346713. Epub 2017 Jul 5.

DOI:10.1080/09593330.2017.1346713
PMID:28643556
Abstract

This paper is focused on development of the metal monolithic structure for total oxidation of toluene at low temperature. The well-adhered catalyst, based on the mixed oxides of manganese and nickel, is washcoated on the Al/AlO plates as metallic support. For the comparison purposes, results observed for the manganese-nickel mixed oxide supported on the metallic monolith are compared with those obtained using powder type of the same catalyst. Prepared manganese-nickel mixed oxides in both configurations show remarkable low-temperature activity for the toluene oxidation. The reaction temperature T corresponding to 50% of the toluene conversion is observed at temperatures of ca. 400-430 K for the powder catalyst and at ca. 450-490 K for the monolith configuration. The appropriate mathematical models, such as one-dimensional (1D) pseudo-homogeneous model of the fixed bed reactor and the 1D heterogeneous model of the metal monolith reactor, are applied to describe and compare catalytic performances of both reactors. Validation of the applied models is performed by comparing experimental data with theoretical predictions. The obtained results confirmed that the reaction over the monolithic structure is kinetically controlled, while in the case of the powder catalyst the reaction rate is influenced by the intraphase diffusion.

摘要

本文聚焦于用于低温下甲苯完全氧化的金属整体结构的开发。基于锰和镍的混合氧化物的附着力良好的催化剂,被涂覆在作为金属载体的Al/AlO板上。为了进行比较,将负载在金属整体上的锰 - 镍混合氧化物的观察结果与使用相同催化剂粉末类型获得的结果进行比较。两种构型中制备的锰 - 镍混合氧化物对甲苯氧化均显示出显著的低温活性。对于粉末催化剂,在约400 - 430 K的温度下观察到甲苯转化率达到50%时对应的反应温度T,而对于整体构型,该温度约为450 - 490 K。应用适当的数学模型,如固定床反应器的一维(1D)拟均相模型和金属整体反应器的1D非均相模型,来描述和比较两个反应器的催化性能。通过将实验数据与理论预测进行比较来对应用模型进行验证。所得结果证实,整体结构上的反应受动力学控制,而对于粉末催化剂,反应速率受相内扩散影响。

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