Comparative study on heterogeneous and homogeneous catalytic ozonation efficiency in micropollutants' removal

Catalytic ozonation was applied for the removal of small concentrations (4 μM) of micropollutants benzotriazole, carbamazepine, p-CBA from aqueous solutions at pH 7. These compounds present different physicochemical characteristics and different kinetic rate constants, when reacting with ozone or hy...

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Main Authors: S. Psaltou, E. Kaprara, M. Mitrakas, A. Zouboulis
Format: Article
Language:English
Published: IWA Publishing 2021-12-01
Series:Aqua
Subjects:
Online Access:http://aqua.iwaponline.com/content/70/8/1121
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author S. Psaltou
E. Kaprara
M. Mitrakas
A. Zouboulis
author_facet S. Psaltou
E. Kaprara
M. Mitrakas
A. Zouboulis
author_sort S. Psaltou
collection DOAJ
description Catalytic ozonation was applied for the removal of small concentrations (4 μM) of micropollutants benzotriazole, carbamazepine, p-CBA from aqueous solutions at pH 7. These compounds present different physicochemical characteristics and different kinetic rate constants, when reacting with ozone or hydroxyl radicals in the ranges of <0.15–3 × 105, 5.2 × 109, and 8.8 × 109 M−1s−1, respectively. Calcite was used as heterogeneous catalyst and its catalytic activity evaluated, by applying (and optimized) different experimental conditions (i.e., pH, temperature, ozone concentration), concerning the removal efficiency of p-CBA. Study of micropollutants' removal showed all examined organic compounds can be sufficiently removed by application of catalytic ozonation either by use of calcite, or by presence of Co(II) or Fe(II) (applied as homogeneous catalysts), while the optimum catalyst between them was found to be calcite. Carbamazepine with kO3 = 3 × 105 M−1s−1 can be easily removed, even by application of single ozonation, while benzotriazole and p-CBA resulted in 50% and 68.2% higher removal after application of catalytic ozonation within 3 min of oxidation reaction, due to acceleration of hydroxyl radicals' production by presence of calcite in the ozonation system. The contribution of hydroxyl radicals in removal of all three micropollutants was evaluated by extraction of Rct and f•OH parameters. HIGHLIGHTS Benzotriazole, carbamazepine and p-CBA were successfully removed by catalytic ozonation.; Among examined catalysts calcite was defined as the best one.; The removal of micropollutants is based on the mechanism of radicals’ production.; Benzotriazole removal was in best agreement with the 1st order kinetic model.; The kinetic model of p-CBA depended on the applicable catalyst.;
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spelling doaj.art-444fa6f095914c8c89d1cc92a23647872022-12-22T04:05:27ZengIWA PublishingAqua2709-80282709-80362021-12-017081121113410.2166/aqua.2021.067067Comparative study on heterogeneous and homogeneous catalytic ozonation efficiency in micropollutants' removalS. Psaltou0E. Kaprara1M. Mitrakas2A. Zouboulis3 Laboratory of Chemical and Environmental Technology, Department of Chemistry, Aristotle University, Thessaloniki 54124, Greece Laboratory of Analytical Chemistry, Department of Chemical Engineering, Aristotle University, Thessaloniki 54124, Greece Laboratory of Analytical Chemistry, Department of Chemical Engineering, Aristotle University, Thessaloniki 54124, Greece Laboratory of Chemical and Environmental Technology, Department of Chemistry, Aristotle University, Thessaloniki 54124, Greece Catalytic ozonation was applied for the removal of small concentrations (4 μM) of micropollutants benzotriazole, carbamazepine, p-CBA from aqueous solutions at pH 7. These compounds present different physicochemical characteristics and different kinetic rate constants, when reacting with ozone or hydroxyl radicals in the ranges of <0.15–3 × 105, 5.2 × 109, and 8.8 × 109 M−1s−1, respectively. Calcite was used as heterogeneous catalyst and its catalytic activity evaluated, by applying (and optimized) different experimental conditions (i.e., pH, temperature, ozone concentration), concerning the removal efficiency of p-CBA. Study of micropollutants' removal showed all examined organic compounds can be sufficiently removed by application of catalytic ozonation either by use of calcite, or by presence of Co(II) or Fe(II) (applied as homogeneous catalysts), while the optimum catalyst between them was found to be calcite. Carbamazepine with kO3 = 3 × 105 M−1s−1 can be easily removed, even by application of single ozonation, while benzotriazole and p-CBA resulted in 50% and 68.2% higher removal after application of catalytic ozonation within 3 min of oxidation reaction, due to acceleration of hydroxyl radicals' production by presence of calcite in the ozonation system. The contribution of hydroxyl radicals in removal of all three micropollutants was evaluated by extraction of Rct and f•OH parameters. HIGHLIGHTS Benzotriazole, carbamazepine and p-CBA were successfully removed by catalytic ozonation.; Among examined catalysts calcite was defined as the best one.; The removal of micropollutants is based on the mechanism of radicals’ production.; Benzotriazole removal was in best agreement with the 1st order kinetic model.; The kinetic model of p-CBA depended on the applicable catalyst.;http://aqua.iwaponline.com/content/70/8/1121advanced oxidation processescatalystscatalytic ozonationmicropollutantsrct valuewater treatment
spellingShingle S. Psaltou
E. Kaprara
M. Mitrakas
A. Zouboulis
Comparative study on heterogeneous and homogeneous catalytic ozonation efficiency in micropollutants' removal
Aqua
advanced oxidation processes
catalysts
catalytic ozonation
micropollutants
rct value
water treatment
title Comparative study on heterogeneous and homogeneous catalytic ozonation efficiency in micropollutants' removal
title_full Comparative study on heterogeneous and homogeneous catalytic ozonation efficiency in micropollutants' removal
title_fullStr Comparative study on heterogeneous and homogeneous catalytic ozonation efficiency in micropollutants' removal
title_full_unstemmed Comparative study on heterogeneous and homogeneous catalytic ozonation efficiency in micropollutants' removal
title_short Comparative study on heterogeneous and homogeneous catalytic ozonation efficiency in micropollutants' removal
title_sort comparative study on heterogeneous and homogeneous catalytic ozonation efficiency in micropollutants removal
topic advanced oxidation processes
catalysts
catalytic ozonation
micropollutants
rct value
water treatment
url http://aqua.iwaponline.com/content/70/8/1121
work_keys_str_mv AT spsaltou comparativestudyonheterogeneousandhomogeneouscatalyticozonationefficiencyinmicropollutantsremoval
AT ekaprara comparativestudyonheterogeneousandhomogeneouscatalyticozonationefficiencyinmicropollutantsremoval
AT mmitrakas comparativestudyonheterogeneousandhomogeneouscatalyticozonationefficiencyinmicropollutantsremoval
AT azouboulis comparativestudyonheterogeneousandhomogeneouscatalyticozonationefficiencyinmicropollutantsremoval