ISSN 1203-8407 © 2007 Science & Technology Network, Inc. J. Adv. Oxid. Technol. Vol. 10, No. 2, 2007 219 Simple Models for the Control of Photo-Fenton by Monitoring H 2 O 2 Jordi Bacardit* , 1 , Isabel Oller 2 , Manuel I. Maldonado 2 , Esther Chamarro 1 , Sixto Malato 2 , and Santiago Esplugas 1 1 Department of Chemical Engineering, University of Barcelona. Martí i Franquès 1, 08028-Barcelona, Spain 2 Plataforma Solar de Almería-CIEMAT, Carretera Senés km 4, 04200-Tabernas (Almería), Spain Abstract: It has been demonstrated that Photo-Fenton process is feasible for the remediation of wastewater containing multiple organic pollutants. In order to promote its industrialization, control strategies have to be defined and tested. The objective of the present work is to describe a mathematical equation that fits the amount of COD abated regarding the dose of H 2 O 2 . UVA Laboratory-scaled and solar up-scaled experiments are compared. Also two H 2 O 2 supply strategies are compared; one in which H 2 O 2 is added at the beginning of an experiment; the second, H 2 O 2 is added in doses through an experiment. According to the results, simple equations have been found to fit experimental COD degraded depending on the amount of H 2 O 2 supplied. There is also a ratio of COD degraded per amount of H 2 O 2 consumed that fits a wide range of operating conditions. The ratio is estimated to be 0.51 (mg O 2 /mg H 2 O 2 ) which can be considered as a stoichiometry of Photo-Fenton process in the current conditions. Introduction Advanced Oxidation Processes (AOPs) are promising methods for the remediation of con- taminated wastewaters containing non-biodegradable organic pollutants (1). They are mostly based on the production of hydroxyl radical HO in water, which is the most powerful oxidising species after fluorine (2.80 V and 3.03 V respectively) (2). The capability of exploiting the high reactivity of HO radicals in driving oxidation processes is suitable for achieving the complete abatement and mineralization of the pollutants through even less reactive species (3). Some of these AOPs, such as Photo-Fenton or Photocatalysis, are based on the interaction of chemical reagents or catalysts with a light source. The present study deals with Photo-Fenton (or photo- assisted Fenton) process (Ph-F). As it is classically described, hydroxyl radicals are produced in this technique by decomposition of hydrogen peroxide when reacting with ferrous ions (Fenton reaction) (4) (Reaction 1). The irradiation with sunlight or an artificial light source of wavelength 180-400 (5) nm or even in the visible spectra (6), increases the rate of contaminant degradation mainly by stimulating the reduction of Fe 3+ to Fe 2+ (5) (Reaction 2). + + + + + HO HO Fe Fe O H 3 2 2 2 (1) + + + + + → + HO H Fe O H Fe 2 2 3 (2) Keywords: Photo-Fenton, COD, efficiency, control, modeling, hydrogen peroxide *Corresponding author; E-mail: bacardit@angel.qui.ub.es As it is generally accepted, hydroxyl radicals formed by these reactions, oxidize the organic species (Reaction 3), generating organic-radical species, which undergo oxidation up to mineralization, dimerize (Reaction 4), or are reduced (Reaction 5) (4). + + i 2 i R O H H R HO (3) (dimer) product 2R i (4) H R Fe Fe R i 3 H 2 i + → + + + + (5) A modern interpretation of Fenton (and photo- Fenton) mechanism, assumes that other oxidizing intermediates such as highly valent iron-complexes (Fe 4+ ) are formed during the oxidation of Fe 2+ to Fe 3+ (Reaction 6 and 7) (7). [ ] + + + + 4 aq 2 2 2 2 2 2 aq Fe O H Fe O H Fe (6) + + + + + HO HO Fe O H Fe 3 aq 2 4 aq (7) Fenton and Photo-Fenton processes are quite complex, and are still matter of discussion. Their mechanisms imply numerous reactions, some of them highly undesirable (8) because they produce an excess of reagent consumption. Some side reactions are commonly represented by Eq. 8 to 11. + + 2 2 2 2 HO O H O H HO (8) 2 2 O H HO HO + (9) + + + + OH Fe Fe HO 3 2 (10) + + + + 3 2 Fe R Fe R (11) Brought to you by | Göteborg University - University of Gothenburg Authenticated Download Date | 1/14/18 12:54 AM