TY - JOUR
T1 - Heterogeneous Fenton oxidation using Fe-ZSM5 catalyst for removal of ibuprofen in wastewater
AU - Adityosulindro, Sandyanto
AU - Julcour, Carine
AU - Barthe, Laurie
N1 - Funding Information:
Financial support by ANR (French National Research Agency) through ANR project “SOFENcoMEM” (ANR- 14-CE04-0006 ) and RISTEKDIKTI (Ministry of Research, Technology and Higher Education of Indonesia) for the scholarship of S. Adityosulindro (No. 2017/E4.4/K/2013 ) are gratefully acknowledged. The authors also thank A. Tißler (Süd-Chemie AG, Clariant) for providing the zeolite, D. Riboul, G. Guittier, M.L. Pern and M.L. de Solan Bethmale (LGC Toulouse) for their help and expert advice on the analytical techniques, J.L. Labat (LGC Toulouse) for the implementation of the experimental set-up and P. Calvet from Nailloux WWTP for wastewater samples.
Publisher Copyright:
© 2018 Elsevier Ltd. All rights reserved.
PY - 2018/10
Y1 - 2018/10
N2 - Heterogeneous Fenton oxidation using Fe-zeolite catalyst (of ZSM5 type) was investigated for the removal of ibuprofen (20 mg/L) in water. In particular, the effects of catalyst concentration, oxidant dosage, temperature, solution pH, and water matrix on pollutant conversion and mineralization were evaluated. The activity of leached iron species in solution was also measured to determine the contribution of the homogeneous reaction. Oxidation rate of ibuprofen obeyed a pseudo-first-order kinetics with respect to the pollutant concentration, and the apparent rate constant increased with catalyst and hydrogen peroxide concentrations in the investigated ranges (1-5 g/L of Fe-zeolite and 0.5-7 times the stoichiometric amount of oxidant). Energy activation of 53 kJ/mol was obtained from Arrhenius plot. However, the mineralization yield was not significantly improved by a too large excess of H2O2 or increase of temperature. In the selected conditions (25 °C, 4.8 g/L of catalyst, 2 times the stoichiometric amount of H2O2), 88% of ibuprofen and 27% of TOC were removed after 3 hours of reaction under "natural" pH conditions. Very low leaching (up to 0.2 mg/L) and negligible activity of leached iron in solution indicated that Fenton reaction was mainly induced by iron species on the catalyst surface. Degradation rate of ibuprofen was slower in wastewater effluent as compared to distilled water, mainly due to alkaline buffering and radical scavenging effects of organic and inorganic compounds present in the matrix. Mono- and multi-hydroxylated ibuprofen adducts were found as main oxidation intermediates -in line with free-radical mechanism- as well as 4-isobutylacetophenone from decarboxylation route.
AB - Heterogeneous Fenton oxidation using Fe-zeolite catalyst (of ZSM5 type) was investigated for the removal of ibuprofen (20 mg/L) in water. In particular, the effects of catalyst concentration, oxidant dosage, temperature, solution pH, and water matrix on pollutant conversion and mineralization were evaluated. The activity of leached iron species in solution was also measured to determine the contribution of the homogeneous reaction. Oxidation rate of ibuprofen obeyed a pseudo-first-order kinetics with respect to the pollutant concentration, and the apparent rate constant increased with catalyst and hydrogen peroxide concentrations in the investigated ranges (1-5 g/L of Fe-zeolite and 0.5-7 times the stoichiometric amount of oxidant). Energy activation of 53 kJ/mol was obtained from Arrhenius plot. However, the mineralization yield was not significantly improved by a too large excess of H2O2 or increase of temperature. In the selected conditions (25 °C, 4.8 g/L of catalyst, 2 times the stoichiometric amount of H2O2), 88% of ibuprofen and 27% of TOC were removed after 3 hours of reaction under "natural" pH conditions. Very low leaching (up to 0.2 mg/L) and negligible activity of leached iron in solution indicated that Fenton reaction was mainly induced by iron species on the catalyst surface. Degradation rate of ibuprofen was slower in wastewater effluent as compared to distilled water, mainly due to alkaline buffering and radical scavenging effects of organic and inorganic compounds present in the matrix. Mono- and multi-hydroxylated ibuprofen adducts were found as main oxidation intermediates -in line with free-radical mechanism- as well as 4-isobutylacetophenone from decarboxylation route.
KW - Advanced oxidation processes
KW - Heterogeneous catalysis
KW - Kinetic study
KW - Pharmaceuticals
KW - Water matrix
KW - Water treatment
UR - http://www.scopus.com/inward/record.url?scp=85053701844&partnerID=8YFLogxK
U2 - 10.1016/j.jece.2018.09.007
DO - 10.1016/j.jece.2018.09.007
M3 - Article
AN - SCOPUS:85053701844
SN - 2213-3437
VL - 6
SP - 5920
EP - 5928
JO - Journal of Environmental Chemical Engineering
JF - Journal of Environmental Chemical Engineering
IS - 5
ER -