Regeneration of activated carbon by fenton and photofenton oxidation for the treatment of phenol wastewater

摘要

Advanced Oxidation Processes have emerged as promising technologies for the recovery of carbons saturated with aromatic molecules, owing to their potency to degrade a wide range of organic pollutants by the generation of very reactive and non selective free hydroxyl radicals. The purpose of this work is to study the adsorption of phenol on activated carbons (ACs) and the consecutive in-situ regeneration of carbon by Fenton oxidation. Two different processes have been carried out: - the first one is based on a complete batch system in order to investigate the influence of Fe2+ and H2O2 concentrations; - the second one consists in a continuous fixed bed adsorption, followed by a batch circulation of the Fenton’s reagent through the saturated AC bed, to examine the efficiency of the real process. Two different activated carbons have been also studied: a both micro- and mesoporous AC (L27) and an only microporous one (S23). In the batch reactor containing a 1 g/L phenol solution, the optimal conditions found for pollutant mineralization in the homogeneous Fenton system (Fe2+ = 10 mmol/L, [H2O2] = 1000 mmol/L, corresponding to 6.5 times the stoechiometric amount for complete mineralization) are not the best for AC regeneration: a continuous reduction of adsorption capacity of L27 from 100% to 23% is observed after 3 oxidations, due to the decrease of both AC weight and surface area. Higher concentration of Fe2+ (20 mmol/L) and lower concentration of H2O2 (2 times the stoechiometry) lead to a 50% recovery of the initial adsorption capacity during at least 4 consecutive cycles for L27, while about 20% or less for S23. In the consecutive continuous adsorption/batch oxidation process, the regeneration efficiency reaches 30% to 40% for L27 after two cycles whatever the feed concentration (0.1 g/L or 1 g/L of phenol) and less than 10% for S23 (0.1 g/L of phenol). During oxidation step, Total Organic Carbon removal is found to reach a limit, probably due to the formation of Fe3+/organic acid complex, hindering Fe2+ regeneration. Such complexes are stable in usual Fenton conditions, but can be destroyed by UV radiation. A photo-Fenton test performed on L27 indeed shows almost complete mineralization and improved recovery of AC adsorption capacity although not complete (56% after two cycles).