Activated carbon as catalyst in wet oxidation of phenol: Effect of the oxidation reaction on the catalyst properties and stability

Abstract

Catalytic wet oxidation (CWO) of phenol has been carried out in a continuous three-phase reactor by using a commercial activated carbon (AC) as catalyst, feeding oxygen as gas phase and an aqueous solution 1000ppm in phenol to the reactor. A stable catalyst under operation conditions is one of the main difficulties to pass up in the catalytic wet oxidation process, so the stability of the activated carbon with the time on stream (TOS) was investigated. To do this the phenol conversion change was analyzed with TOS and results were contrasted to the change of the physicochemical properties of the AC with the TOS. Gas adsorption/desorption, TPD, XPS and SEM measurements were applied to the AC taken from the reactor after several TOS values. A significant reduction of the micro-pore volume and BET surface area of the catalyst was observed with TOS. However, as reaction proceeded the external surface area and the total amount of oxygen surface group increased. Moreover, regeneration of the initial catalyst properties was done by washing with water saturated in oxygen, at the reaction conditions or by heating in N2 atmosphere at 450, 700 and 900°C. The total micro-pore volume and internal surface area of the catalyst were not recovered by the regeneration process, probably due to blockage of the narrow micropores by pyrolytic carbon produced during the first step of the wet oxidation process.