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
Research output: Journal contributions › Journal articles › Research › peer-review
Standard
In: The Science of The Total Environment, Vol. 527-528, 15.09.2015, p. 232-245.
Research output: Journal contributions › Journal articles › Research › peer-review
Harvard
APA
Vancouver
Bibtex
}
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 -