Degradation of 5-FU by means of advanced (photo)oxidation processes: UV/H2O2, UV/Fe(2+)/H2O2 and UV/TiO2 - Comparison of transformation products, ready biodegradability and toxicity

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Degradation of 5-FU by means of advanced (photo)oxidation processes: UV/H2O2, UV/Fe(2+)/H2O2 and UV/TiO2 - Comparison of transformation products, ready biodegradability and toxicity. / Lutterbeck, Carlos Alexandre; Wilde, Marcelo Luís; Baginska, Ewelina et al.
in: The Science of The Total Environment, Jahrgang 527-528, 15.09.2015, S. 232-245.

Publikation: Beiträge in ZeitschriftenZeitschriftenaufsätzeForschungbegutachtet

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@article{836d127a193c4b8cbb40bf7df9ba722e,
title = "Degradation of 5-FU by means of advanced (photo)oxidation processes: UV/H2O2, UV/Fe(2+)/H2O2 and UV/TiO2 - Comparison of transformation products, ready biodegradability and toxicity",
abstract = "The present study investigates the degradation of the antimetabolite 5-fluorouracil (5-FU) by three different advanced photo oxidation processes: UV/H2O2, UV/Fe(2+)/H2O2 and UV/TiO2. Prescreening experiments varying the H2O2 and TiO2 concentrations were performed in order to set the best catalyst concentrations in the UV/H2O2 and UV/TiO2 experiments, whereas the UV/Fe(2+)/H2O2 process was optimized varying the pH, Fe(2+) and H2O2 concentrations by means of the Box-Behnken design (BBD). 5-FU was quickly removed in all the irradiation experiments. The UV/Fe(2+)/H2O2 and UV/TiO2 processes achieved the highest degree of mineralization, whereas the lowest one resulted from the UV/H2O2 treatment. Six transformation products were formed during the advanced (photo)oxidation processes and identified using low and high resolution mass spectrometry. Most of them were formed and further eliminated during the reactions. The parent compound of 5-FU was not biodegraded, whereas the photolytic mixture formed in the UV/H2O2 treatment after 256min showed a noticeable improvement of the biodegradability in the closed bottle test (CBT) and was nontoxic towards Vibrio fischeri. In silico predictions showed positive alerts for mutagenic and genotoxic effects of 5-FU. In contrast, several of the transformation products (TPs) generated along the processes did not provide indications for mutagenic or genotoxic activity. One exception was TP with m/z 146 with positive alerts in several models of bacterial mutagenicity which could demand further experimental testing. Results demonstrate that advanced treatment can eliminate parent compounds and its toxicity. However, transformation products formed can still be toxic. Therefore toxicity screening after advanced treatment is recommendable.",
keywords = "Chemistry, 5-Fluorouracil, Photodegradation, Transformation product, Sustainability Science",
author = "Lutterbeck, {Carlos Alexandre} and Wilde, {Marcelo Lu{\'i}s} and Ewelina Baginska and Christoph Leder and Machado, {{\^E}nio Leandro} and Klaus K{\"u}mmerer",
note = "Copyright {\textcopyright} 2015 Elsevier B.V. All rights reserved.",
year = "2015",
month = sep,
day = "15",
doi = "10.1016/j.scitotenv.2015.04.111",
language = "English",
volume = "527-528",
pages = "232--245",
journal = "The Science of The Total Environment",
issn = "0048-9697",
publisher = "Elsevier B.V.",

}

RIS

TY - JOUR

T1 - Degradation of 5-FU by means of advanced (photo)oxidation processes

T2 - UV/H2O2, UV/Fe(2+)/H2O2 and UV/TiO2 - Comparison of transformation products, ready biodegradability and toxicity

AU - Lutterbeck, Carlos Alexandre

AU - Wilde, Marcelo Luís

AU - Baginska, Ewelina

AU - Leder, Christoph

AU - Machado, Ênio Leandro

AU - Kümmerer, Klaus

N1 - Copyright © 2015 Elsevier B.V. All rights reserved.

PY - 2015/9/15

Y1 - 2015/9/15

N2 - The present study investigates the degradation of the antimetabolite 5-fluorouracil (5-FU) by three different advanced photo oxidation processes: UV/H2O2, UV/Fe(2+)/H2O2 and UV/TiO2. Prescreening experiments varying the H2O2 and TiO2 concentrations were performed in order to set the best catalyst concentrations in the UV/H2O2 and UV/TiO2 experiments, whereas the UV/Fe(2+)/H2O2 process was optimized varying the pH, Fe(2+) and H2O2 concentrations by means of the Box-Behnken design (BBD). 5-FU was quickly removed in all the irradiation experiments. The UV/Fe(2+)/H2O2 and UV/TiO2 processes achieved the highest degree of mineralization, whereas the lowest one resulted from the UV/H2O2 treatment. Six transformation products were formed during the advanced (photo)oxidation processes and identified using low and high resolution mass spectrometry. Most of them were formed and further eliminated during the reactions. The parent compound of 5-FU was not biodegraded, whereas the photolytic mixture formed in the UV/H2O2 treatment after 256min showed a noticeable improvement of the biodegradability in the closed bottle test (CBT) and was nontoxic towards Vibrio fischeri. In silico predictions showed positive alerts for mutagenic and genotoxic effects of 5-FU. In contrast, several of the transformation products (TPs) generated along the processes did not provide indications for mutagenic or genotoxic activity. One exception was TP with m/z 146 with positive alerts in several models of bacterial mutagenicity which could demand further experimental testing. Results demonstrate that advanced treatment can eliminate parent compounds and its toxicity. However, transformation products formed can still be toxic. Therefore toxicity screening after advanced treatment is recommendable.

AB - The present study investigates the degradation of the antimetabolite 5-fluorouracil (5-FU) by three different advanced photo oxidation processes: UV/H2O2, UV/Fe(2+)/H2O2 and UV/TiO2. Prescreening experiments varying the H2O2 and TiO2 concentrations were performed in order to set the best catalyst concentrations in the UV/H2O2 and UV/TiO2 experiments, whereas the UV/Fe(2+)/H2O2 process was optimized varying the pH, Fe(2+) and H2O2 concentrations by means of the Box-Behnken design (BBD). 5-FU was quickly removed in all the irradiation experiments. The UV/Fe(2+)/H2O2 and UV/TiO2 processes achieved the highest degree of mineralization, whereas the lowest one resulted from the UV/H2O2 treatment. Six transformation products were formed during the advanced (photo)oxidation processes and identified using low and high resolution mass spectrometry. Most of them were formed and further eliminated during the reactions. The parent compound of 5-FU was not biodegraded, whereas the photolytic mixture formed in the UV/H2O2 treatment after 256min showed a noticeable improvement of the biodegradability in the closed bottle test (CBT) and was nontoxic towards Vibrio fischeri. In silico predictions showed positive alerts for mutagenic and genotoxic effects of 5-FU. In contrast, several of the transformation products (TPs) generated along the processes did not provide indications for mutagenic or genotoxic activity. One exception was TP with m/z 146 with positive alerts in several models of bacterial mutagenicity which could demand further experimental testing. Results demonstrate that advanced treatment can eliminate parent compounds and its toxicity. However, transformation products formed can still be toxic. Therefore toxicity screening after advanced treatment is recommendable.

KW - Chemistry

KW - 5-Fluorouracil

KW - Photodegradation

KW - Transformation product

KW - Sustainability Science

UR - http://www.scopus.com/inward/record.url?scp=84928881610&partnerID=8YFLogxK

UR - https://www.mendeley.com/catalogue/d315bd5c-44b8-3918-b093-0f908709997c/

U2 - 10.1016/j.scitotenv.2015.04.111

DO - 10.1016/j.scitotenv.2015.04.111

M3 - Journal articles

C2 - 25965036

VL - 527-528

SP - 232

EP - 245

JO - The Science of The Total Environment

JF - The Science of The Total Environment

SN - 0048-9697

ER -

DOI

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