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Open Access Green möglich sobald Postprint bei der ZB eingereicht worden ist.
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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Publikationstyp
Artikel: Journalartikel
Dokumenttyp
Wissenschaftlicher Artikel
Schlagwörter
Pharmaceutical Drug Diclofenac; Waste-water; Manganese Oxide; Surface Waters; Acidic Pharmaceuticals; Contaminated Aquifers; Organic Contaminants; Aquatic Environment; Clofibric Acid; Oxidation
ISSN (print) / ISBN
0013-936X
e-ISSN
1520-5851
Zeitschrift
Environmental Science & Technology
Quellenangaben
Band: 50,
Heft: 20,
Seiten: 10933-10942
Verlag
ACS
Verlagsort
Washington, DC
Nichtpatentliteratur
Publikationen
Begutachtungsstatus
Peer reviewed
Institut(e)
Institute of Groundwater Ecology (IGOE)