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Visible-Light Activation of Persulfate or H(2)O(2) by Fe(2)O(3)/TiO(2) Immobilized on Glass Support for Photocatalytic Removal of Amoxicillin: Mechanism, Transformation Products, and Toxicity Assessment
Fe(2)O(3)/TiO(2) nanocomposites were fabricated via a facile impregnation/calcination technique employing different amounts iron (III) nitrate onto commercial TiO(2) (P25 Aeroxide). The as-prepared Fe(2)O(3)/TiO(2) nanocomposites were characterized by X-ray diffraction (XRD), Raman spectroscopy (RS)...
Autores principales: | , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
MDPI
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9738309/ https://www.ncbi.nlm.nih.gov/pubmed/36500951 http://dx.doi.org/10.3390/nano12234328 |
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author | dela Rosa, Francis M. Popović, Marin Papac Zjačić, Josipa Radić, Gabrijela Kraljić Roković, Marijana Kovačić, Marin Farré, María José Genorio, Boštjan Lavrenčič Štangar, Urška Kušić, Hrvoje Lončarić Božić, Ana Petrović, Mira |
author_facet | dela Rosa, Francis M. Popović, Marin Papac Zjačić, Josipa Radić, Gabrijela Kraljić Roković, Marijana Kovačić, Marin Farré, María José Genorio, Boštjan Lavrenčič Štangar, Urška Kušić, Hrvoje Lončarić Božić, Ana Petrović, Mira |
author_sort | dela Rosa, Francis M. |
collection | PubMed |
description | Fe(2)O(3)/TiO(2) nanocomposites were fabricated via a facile impregnation/calcination technique employing different amounts iron (III) nitrate onto commercial TiO(2) (P25 Aeroxide). The as-prepared Fe(2)O(3)/TiO(2) nanocomposites were characterized by X-ray diffraction (XRD), Raman spectroscopy (RS), scanning electron microscopy/energy-dispersive spectroscopy (SEM/EDXS), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller analysis (BET), electron impedance spectroscopy (EIS), photoluminescence spectroscopy (PL), and diffuse reflectance spectroscopy (DRS). As a result, 5% (w/w) Fe(2)O(3)/TiO(2) achieved the highest photocatalytic activity in the slurry system and was successfully immobilized on glass support. Photocatalytic activity under visible-light irradiation was assessed by treating pharmaceutical amoxicillin (AMX) in the presence and absence of additional oxidants: hydrogen peroxide (H(2)O(2)) and persulfate salts (PS). The influence of pH and PS concentration on AMX conversion rate was established by means of statistical planning and response surface modeling. Results revealed optimum conditions of [S(2)O(8)(2−)] = 1.873 mM and pH = 4.808; these were also utilized in presence of H(2)O(2) instead of PS in long-term tests. The fastest AMX conversion possessing a zero-order rate constant of 1.51 × 10(−7) M·min(−1) was achieved with the photocatalysis + PS system. The AMX conversion pathway was established, and the evolution/conversion of formed intermediates was correlated with the changes in toxicity toward Vibrio fischeri. Reactive oxygen species (ROS) scavenging was also utilized to investigate the AMX conversion mechanism, revealing the major contribution of photogenerated h(+) in all processes. |
format | Online Article Text |
id | pubmed-9738309 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | MDPI |
record_format | MEDLINE/PubMed |
spelling | pubmed-97383092022-12-11 Visible-Light Activation of Persulfate or H(2)O(2) by Fe(2)O(3)/TiO(2) Immobilized on Glass Support for Photocatalytic Removal of Amoxicillin: Mechanism, Transformation Products, and Toxicity Assessment dela Rosa, Francis M. Popović, Marin Papac Zjačić, Josipa Radić, Gabrijela Kraljić Roković, Marijana Kovačić, Marin Farré, María José Genorio, Boštjan Lavrenčič Štangar, Urška Kušić, Hrvoje Lončarić Božić, Ana Petrović, Mira Nanomaterials (Basel) Article Fe(2)O(3)/TiO(2) nanocomposites were fabricated via a facile impregnation/calcination technique employing different amounts iron (III) nitrate onto commercial TiO(2) (P25 Aeroxide). The as-prepared Fe(2)O(3)/TiO(2) nanocomposites were characterized by X-ray diffraction (XRD), Raman spectroscopy (RS), scanning electron microscopy/energy-dispersive spectroscopy (SEM/EDXS), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller analysis (BET), electron impedance spectroscopy (EIS), photoluminescence spectroscopy (PL), and diffuse reflectance spectroscopy (DRS). As a result, 5% (w/w) Fe(2)O(3)/TiO(2) achieved the highest photocatalytic activity in the slurry system and was successfully immobilized on glass support. Photocatalytic activity under visible-light irradiation was assessed by treating pharmaceutical amoxicillin (AMX) in the presence and absence of additional oxidants: hydrogen peroxide (H(2)O(2)) and persulfate salts (PS). The influence of pH and PS concentration on AMX conversion rate was established by means of statistical planning and response surface modeling. Results revealed optimum conditions of [S(2)O(8)(2−)] = 1.873 mM and pH = 4.808; these were also utilized in presence of H(2)O(2) instead of PS in long-term tests. The fastest AMX conversion possessing a zero-order rate constant of 1.51 × 10(−7) M·min(−1) was achieved with the photocatalysis + PS system. The AMX conversion pathway was established, and the evolution/conversion of formed intermediates was correlated with the changes in toxicity toward Vibrio fischeri. Reactive oxygen species (ROS) scavenging was also utilized to investigate the AMX conversion mechanism, revealing the major contribution of photogenerated h(+) in all processes. MDPI 2022-12-05 /pmc/articles/PMC9738309/ /pubmed/36500951 http://dx.doi.org/10.3390/nano12234328 Text en © 2022 by the authors. https://creativecommons.org/licenses/by/4.0/Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Article dela Rosa, Francis M. Popović, Marin Papac Zjačić, Josipa Radić, Gabrijela Kraljić Roković, Marijana Kovačić, Marin Farré, María José Genorio, Boštjan Lavrenčič Štangar, Urška Kušić, Hrvoje Lončarić Božić, Ana Petrović, Mira Visible-Light Activation of Persulfate or H(2)O(2) by Fe(2)O(3)/TiO(2) Immobilized on Glass Support for Photocatalytic Removal of Amoxicillin: Mechanism, Transformation Products, and Toxicity Assessment |
title | Visible-Light Activation of Persulfate or H(2)O(2) by Fe(2)O(3)/TiO(2) Immobilized on Glass Support for Photocatalytic Removal of Amoxicillin: Mechanism, Transformation Products, and Toxicity Assessment |
title_full | Visible-Light Activation of Persulfate or H(2)O(2) by Fe(2)O(3)/TiO(2) Immobilized on Glass Support for Photocatalytic Removal of Amoxicillin: Mechanism, Transformation Products, and Toxicity Assessment |
title_fullStr | Visible-Light Activation of Persulfate or H(2)O(2) by Fe(2)O(3)/TiO(2) Immobilized on Glass Support for Photocatalytic Removal of Amoxicillin: Mechanism, Transformation Products, and Toxicity Assessment |
title_full_unstemmed | Visible-Light Activation of Persulfate or H(2)O(2) by Fe(2)O(3)/TiO(2) Immobilized on Glass Support for Photocatalytic Removal of Amoxicillin: Mechanism, Transformation Products, and Toxicity Assessment |
title_short | Visible-Light Activation of Persulfate or H(2)O(2) by Fe(2)O(3)/TiO(2) Immobilized on Glass Support for Photocatalytic Removal of Amoxicillin: Mechanism, Transformation Products, and Toxicity Assessment |
title_sort | visible-light activation of persulfate or h(2)o(2) by fe(2)o(3)/tio(2) immobilized on glass support for photocatalytic removal of amoxicillin: mechanism, transformation products, and toxicity assessment |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9738309/ https://www.ncbi.nlm.nih.gov/pubmed/36500951 http://dx.doi.org/10.3390/nano12234328 |
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