Catalytic wet peroxide oxidation of phenol with a Fe/active carbon catalyst

Abstract A Fe on activated carbon catalyst has been prepared and tested for phenol oxidation with H 2 O 2 in aqueous solution at low concentration (100 mg/L). Working at 50 °C, initial pH 3 and a dose of H 2 O 2 corresponding to the stoichiometric amount (500 mg/L) complete removal of phenol and a high TOC reduction (around 85%) has been reached. Oxidation of phenol gives rise to highly toxic aromatic intermediates which finally disappear completely evolving to short-chain organic acids. Some of these last showed to be fairly resistant to oxidation being responsible for the residual TOC. In long-term continuous experiments the catalyst undergoes a significant loss of activity in a relatively short term (20–25 h) due to Fe leaching, this being related with the amount of oxalic acid produced. Deactivation may also be caused by active sites blockage due to polymeric deposits on whose formation some evidences were found. Washing with 1N NaOH solution allows to recover the activity although complete restoration was not achieved.

[1]  J. Barrault,et al.  Active iron species in the catalytic wet peroxide oxidation of phenol over pillared clays containing iron , 2003 .

[2]  F. Rodríguez-Reinoso,et al.  The role of carbon materials in heterogeneous catalysis , 1998 .

[3]  G. Eisenberg Colorimetric Determination of Hydrogen Peroxide , 1943 .

[4]  N. Papayannakos,et al.  Catalytic wet peroxide oxidation over mixed (Al-Fe) pillared clays , 2000 .

[5]  Juin-Yih Lai,et al.  Fe (III) supported on resin as effective catalyst for the heterogeneous oxidation of phenol in aqueous solution. , 2005, Chemosphere.

[6]  H. Debellefontaine,et al.  Influence de Quelques Paramètres Opératoires Sur l'Oxydation du Phénol par le Peroxyde d'Hydrogène en Présence D'une Zéolithe Fe-ZSM-5 Dependency on some Operating Parameters During Wet Oxidation of Phenol by Hydrogen Peroxide with Fe-ZSM-5 Zeolite , 2000 .

[7]  Carmen Teodosiu,et al.  Catalytic wet peroxide oxidation of phenol over Fe-exchanged pillared beidellite. , 2003, Water research.

[8]  H. Debellefontaine,et al.  Wet oxidation of phenol by hydrogen peroxide using heterogeneous catalysis Fe-ZSM-5: a promising catalyst , 1996 .

[9]  Xavier Domènech,et al.  Removal of organic contaminants in paper pulp treatment effluents under Fenton and photo-Fenton conditions , 2002 .

[10]  Piero Salvadori,et al.  A preliminary study on iron species as heterogeneous catalysts for the degradation of linear alkylbenzene sulphonic acids by H2O2 , 2002 .

[11]  F. Carrasco-Marín,et al.  Changes in surface chemistry of activated carbons by wet oxidation , 2000 .

[12]  Frank Leung Yuk Lam,et al.  Copper/MCM-41 as catalyst for photochemically enhanced oxidation of phenol by hydrogen peroxide , 2001 .

[13]  F. García-Ochoa,et al.  Route of the catalytic oxidation of phenol in aqueous phase , 2002 .

[14]  Bao-Lian Su,et al.  Iron, cobalt or nickel substituted MCM-41 molecular sieves for oxidation of hydrocarbons , 2001 .

[15]  J. J. Rodríguez,et al.  Influence of Surface Composition and Pore Structure on Cr(III) Adsorption onto Activated Carbons , 2002 .

[16]  J. Figueiredo,et al.  Modification of the surface chemistry of activated carbons , 1999 .

[17]  J. Foussard,et al.  Wet oxidation of phenol by hydrogen peroxide: The key role of pH on the catalytic behaviour of Fe-ZSM-5 , 1997 .

[18]  E. Sandell Colorimetric Determination of Traces of Metals , 1944 .

[19]  D. Cooney,et al.  Activated carbon catalyzes reactions of phenolics during liquid‐phase adsorption , 1994 .

[20]  A. Pintar Catalytic processes for the purification of drinking water and industrial effluents , 2003 .

[21]  M. Dore,et al.  Oxydation des phenols par le peroxyde d'hydrogene en milieu aqueux en presence de fer supporte sur alumine , 1990 .

[22]  Jing Guo,et al.  Catalytic Wet Oxidation of Phenol by Hydrogen Peroxide over Pillared Clay Catalyst , 2003 .

[23]  J. Casas,et al.  Evolution of toxicity upon wet catalytic oxidation of phenol. , 2004, Environmental science & technology.