| As an important approach for the wastewater treatment, catalytic wet oxidation (CWO) in packed bed reactors has drawn significant attention in the chemical and petrochemical industries. A packed-bed reactor, especially in the upflow mode of operation, has been shown to be more suitable for the CWO process than other reactor types. CWO of phenol in aqueous phase is studied in this work over a newly developed Al-Fe pillared clay catalyst. This catalyst has shown potential for wastewater treatment, as it reduces the reaction temperature and pressure and provides better resistant to deactivation. For reactor design and scale-up, the interactions between the involved reaction kinetics, hydrodynamics, interphase and intraparticle transport in the catalytic packed bed at different reaction conditions needs to be addressed. The goal is to get complete mineralization of phenol at mild conditions and to identify the corresponding operating conditions.; In the experiment part, pillared clay catalyst performance for wastewater treatment (phenol removal) was investigated in both batch and packed bed reactors. Batch experiments, using a basket reactor, were performed to identify the suitable operating conditions, and to derive the apparent reaction kinetics for phenol removal. Appropriate kinetic models were derived and used to predict packed bed performance. The performance of the pillared clay catalyst for phenol oxidation in a packed bed process was investigated with co-current downflow and upflow. Under rather mild conditions, the Al-Fe pillared clay catalyst can achieve total elimination of phenol and significant mineralization (80--100%) of total organic carbon (TOC). The catalyst deactivation is investigated via three different detection methods: particle pore BET analysis, scanning electron microscopy (SEM), and inductively coupled plasma (ICP).; In the modeling part, a suitable reactor scale model is evaluated and extended to predict the performance of packed-bed reactors under employed conditions. The effects of key parameters, such as extent of liquid-solid contacting, gas/liquid limitation, and mass transfer resistance, have been investigated. The model is modified to account for the volatilization of the solvent. Such a modeling strategy is aimed to provide a tool for further evaluation of the new catalyst design and various operating conditions. |
