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Open Access Green as soon as Postprint is submitted to ZB.
Exploring trends of C and N isotope fractionation to trace transformation reactions of diclofenac in natural and engineered systems.
Environ. Sci. Technol. 50, 10933-10942 (2016)
Although diclofenac ranks among the most frequently detected pharmaceuticals in the urban water cycle, its environmental transformation reactions remain imperfectly understood. Biodegradation-induced changes in 15N/14N ratios (εN = -7.1‰ ± 0.4‰) have indicated that compound-specific isotope analysis (CSIA) may detect diclofenac degradation. This singular observation warrants exploration for further transformation reactions. The present study surveys carbon and nitrogen isotope fractionation in other environmental and engineered transformation reactions of diclofenac. While carbon isotope fractionation was generally small, observed nitrogen isotope fractionation in degradation by MnO2 (εN = -7.3‰ ± 0.3‰), photolysis (εN = +1.9‰ ± 0.1‰), and ozonation (εN = +1.5‰ ± 0.2‰) revealed distinct trends for different oxidative transformation reactions. The small, secondary isotope effect associated with ozonation suggests an attack of O3 in a molecular position distant from the N atom. Model reactants for outer-sphere single electron transfer generated large inverse nitrogen isotope fractionation (εN = +5.7‰ ± 0.3‰), ruling out this mechanism for biodegradation and transformation by MnO2. In a river model, isotope fractionation-derived degradation estimates agreed well with concentration mass balances, providing a proof-of-principle validation for assessing micropollutant degradation in river sediment. Our study highlights the prospect of combining CSIA with transformation product analysis for a better assessment of transformation reactions within the environmental life of diclofenac.
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Publication type
Article: Journal article
Document type
Scientific Article
Keywords
Pharmaceutical Drug Diclofenac; Waste-water; Manganese Oxide; Surface Waters; Acidic Pharmaceuticals; Contaminated Aquifers; Organic Contaminants; Aquatic Environment; Clofibric Acid; Oxidation
Language
Publication Year
2016
HGF-reported in Year
2016
ISSN (print) / ISBN
0013-936X
e-ISSN
1520-5851
Quellenangaben
Volume: 50,
Issue: 20,
Pages: 10933-10942
Publisher
ACS
Publishing Place
Washington, DC
Reviewing status
Peer reviewed
Institute(s)
Institute of Groundwater Ecology (IGOE)
POF-Topic(s)
20403 - Sustainable Water Management
Research field(s)
Environmental Sciences
PSP Element(s)
G-504390-001
PubMed ID
27635778
WOS ID
WOS:000385907200019
Scopus ID
84991744758
Erfassungsdatum
2016-10-17