Removal of antibiotics by an integrated process coupling photocatalysis and biological treatment - Case of tetracycline and tylosin

Abstract Much attention has been recently devoted to the fate of pharmaceutically active compounds such as antibiotics in soil and water. Among them, tetracycline (TC) and tylosin (TYL) antibiotics were shown to be poorly biodegradable and toxic for microorganisms. The question of their fate in the environment has to be clearly identified in order to prevent any environmental contamination and to avoid generating antibioresistant strains. Hybrid processes involving a physico-chemical pre-treatment like photocatalysis coupled to a biological treatment have been considered for their removal. Prior to a biological treatment, pre-treatment of both antibiotics by photocatalysis was considered in this work. To ensure a significant residual organic content for the biological treatment, an irradiation time of 2 h was considered. A decrease of the residual amount of antibiotics contained in the irradiated solutions was recorded, which can be related to an “inherent” biodegradation since these residual concentrations were below their inhibitory thresholds, 18 and 9 mg l −1 for TC and TYL. The absence of biodegradability of TC by-products was noted because of their toxicity (EC 50 50 50  = 36%) after irradiation.

[1]  S. Kenfack,et al.  An innovative coupled solar-biological system at field pilot scale for the treatment of biorecalcitrant pollutants , 2003 .

[2]  F. Bordin Photochemical and photobiological properties of furocoumarins and homologues drugs , 1999 .

[3]  G. Peñuela,et al.  Photocatalytic oxidation of the antibiotic tetracycline on TiO2 and ZnO suspensions , 2009 .

[4]  B. Halling‐Sørensen,et al.  Acute and chronic toxicity of veterinary antibiotics to Daphnia magna. , 2000, Chemosphere.

[5]  C. Chauvin,et al.  A survey of group-level antibiotic prescriptions in pig production in France. , 2002, Preventive veterinary medicine.

[6]  X. Doménech,et al.  Evaluation of the intermediates generated during the degradation of Diuron and Linuron herbicides by the photo-Fenton reaction , 2007 .

[7]  C. Zaror,et al.  Degradation and inactivation of tetracycline by TiO2 photocatalysis , 2006 .

[8]  D. Wolbert,et al.  Photocatalytic degradation of a triazole pesticide, cyproconazole, in water , 2007 .

[9]  C. Pulgarin,et al.  Degradation of a biorecalcitrant dye precursor present in industrial wastewaters by a new integrated iron(III) photoassisted-biological treatment , 2003 .

[10]  Wei Chen,et al.  Mechanisms for strong adsorption of tetracycline to carbon nanotubes: a comparative study using activated carbon and graphite as adsorbents. , 2009, Environmental science & technology.

[11]  M. Bouchy,et al.  Decolourization of Textile Industry Wastewater by the Photocatalytic Degradation Process , 2001 .

[12]  A. Amrane,et al.  Evaluation of the toxicity of veterinary antibiotics on activated sludge using modified Sturm tests - application to tetracycline and tylosine antibiotics. , 2009 .

[13]  M. Bayramoğlu,et al.  The degradation of an azo dye in a batch slurry photocatalytic reactor , 2008 .

[14]  J. Blanco,et al.  Photocatalytic treatment of water-soluble pesticides by photo-Fenton and TiO2 using solar energy , 2002 .

[15]  R. Sturm Biodegradability of nonionic surfactants: Screening test for predicting rate and ultimate biodegradation , 1973, Journal of the American Oil Chemists' Society.

[16]  D. Mantzavinos,et al.  Removal of residual pharmaceuticals from aqueous systems by advanced oxidation processes. , 2009, Environment international.

[17]  S. Jørgensen,et al.  Occurrence, fate and effects of pharmaceutical substances in the environment--a review. , 1998, Chemosphere.

[18]  D. Wolbert,et al.  Gas phase photocatalysis and liquid phase photocatalysis: Interdependence and influence of substrate concentration and photon flow on degradation reaction kinetics , 2008 .

[19]  T. Heberer Occurrence, fate, and removal of pharmaceutical residues in the aquatic environment: a review of recent research data. , 2002, Toxicology letters.

[20]  A. Amrane,et al.  Biodegradation and biosorption of tetracycline and tylosin antibiotics in activated sludge system , 2009 .

[21]  C. Pulgarin,et al.  Strategy for the coupling of photochemical and biological flow reactors useful in mineralization of biorecalcitrant industrial pollutants , 1999 .

[22]  Ammar Houas,et al.  Influence of chemical structure of dyes, of pH and of inorganic salts on their photocatalytic degradation by TiO2 comparison of the efficiency of powder and supported TiO2 , 2003 .

[23]  C. Galindo,et al.  Photooxidation of the phenylazonaphthol AO20 on TIO2: kinetic and mechanistic investigations. , 2001, Chemosphere.

[24]  C. Pulgarin,et al.  Relationships between physicochemical properties and photoreactivity of four biorecalcitrant phenylurea herbicides in aqueous TiO2 suspension , 2002 .

[25]  S. Brosillon,et al.  Influence of ionic strength in the adsorption and during photocatalysis of reactive black 5 azo dye on TiO2 coated on non woven paper with SiO2 as a binder. , 2008, Journal of hazardous materials.

[26]  Bent Halling-Sørensen,et al.  Bacterial antibiotic resistance levels in Danish farmland as a result of treatment with pig manure slurry. , 2003, Environment international.

[27]  P. Jjemba The potential impact of veterinary and human therapeutic agents in manure and biosolids on plants grown on arable land: a review , 2002 .

[28]  A. Amrane,et al.  Integrated Process for Degradation of Amitrole in Wastewaters: Photocatalysis/Biodegradation , 2007 .

[29]  R. Augusti,et al.  Monitoring the degradation of tetracycline by ozone in aqueous medium via atmospheric pressure ionization mass spectrometry , 2007, Journal of the American Society for Mass Spectrometry.

[30]  Santiago Esplugas,et al.  Ozonation and advanced oxidation technologies to remove endocrine disrupting chemicals (EDCs) and pharmaceuticals and personal care products (PPCPs) in water effluents. , 2007, Journal of hazardous materials.

[31]  David F. Ollis,et al.  Integration of chemical and biological oxidation processes for water treatment: Review and recommendations , 1995 .

[32]  C. Pulgarin,et al.  Chemical (photo-activated) coupled biological homogeneous degradation of p-nitro-o-toluene-sulfonic acid in a flow reactor , 1997 .

[33]  M. I. Maldonado,et al.  Detoxification of wastewater containing five common pesticides by solar AOPs–biological coupled system , 2007 .

[34]  N. Yamashita,et al.  Photodegradation of pharmaceuticals and personal care products during UV and UV/H2O2 treatments. , 2009, Chemosphere.

[35]  Keiichi Tanaka,et al.  Photocatalytic degradation of commercial azo dyes , 2000 .

[36]  Y. Segura,et al.  Heterogeneous photo-Fenton treatment for the reduction of pharmaceutical contamination in Madrid rivers and ecotoxicological evaluation by a miniaturized fern spores bioassay. , 2010, Chemosphere.

[37]  R. Nogueira,et al.  Degradation of tetracycline by photo-Fenton process - Solar irradiation and matrix effects , 2007 .

[38]  S. Brosillon,et al.  Photocatalytic degradation of azo-dyes reactive black 5 and reactive yellow 145 in water over a newly deposited titanium dioxide , 2005 .

[39]  A P Trinci,et al.  A kinetic study of the growth of Aspergillus nidulans and other fungi. , 1969, Journal of general microbiology.

[40]  A. Boxall,et al.  A global perspective on the use, sales, exposure pathways, occurrence, fate and effects of veterinary antibiotics (VAs) in the environment. , 2006, Chemosphere.

[41]  B. Halling-Sørensen,et al.  Reduced Antimicrobial Potencies of Oxytetracycline, Tylosin, Sulfadiazin, Streptomycin, Ciprofloxacin, and Olaquindox Due to Environmental Processes , 2003, Archives of environmental contamination and toxicology.

[42]  C. Galindo,et al.  Photodegradation of the aminoazobenzene acid orange 52 by three advanced oxidation processes: UV/H2O2, UV/TiO2 and VIS/TiO2: Comparative mechanistic and kinetic investigations , 2000 .

[43]  H. Djelal,et al.  Innovative integrated process for the treatment of azo dyes: coupling of photocatalysis and biological treatment , 2008 .

[44]  J. Araña,et al.  Comparative study of MTBE photocatalytic degradation with TiO2 and Cu-TiO2 , 2008 .

[45]  Marco Bertelli,et al.  Kinetic analysis on the combined use of photocatalysis, H2O2 photolysis, and sonolysis in the degradation of methyl tert-butyl ether , 2004 .

[46]  B. Halling‐Sørensen,et al.  Dissipation and effects of chlortetracycline and tylosin in two agricultural soils: A field‐scale study in southern Denmark , 2005, Environmental toxicology and chemistry.

[47]  C. Pulgarin,et al.  Recent developments in the coupling of photoassisted and aerobic biological processes for the treatment of biorecalcitrant compounds , 2002 .

[48]  H. Heipieper,et al.  Degradation of macrolide antibiotics by ozone: a mechanistic case study with clarithromycin. , 2006, Chemosphere.