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C & N isotope analysis of diclofenac to distinguish oxidative and reductive transformation and to track commercial products.
Environ. Sci. Technol. 48, 2312-2320 (2014)
Although diclofenac is frequently found in aquatic systems, its degradability in the environment remains imperfectly understood. On the one hand, evidence from concentration analysis alone is inconclusive if an unknown hydrology impedes a distinction between degradation and dilution. On the other hand, not all transformation products may be detectable. As a new approach, we therefore developed GC-IRMS (gas chromatography-isotope-ratio mass-spectrometry) analysis for carbon and nitrogen isotope measurements of diclofenac. The method uses a derivatization step that can be conducted either online or offline, for optimized throughput or sensitivity, respectively. In combination with on-column injection, the latter method enables determination of diclofenac isotope ratios down to the sub-μgL(-1) range in environmental samples. Degradation in an aerobic sediment-water system showed strong nitrogen isotope fractionation (εN = -7.1‰), whereas reductive diclofenac dechlorination was associated with significant carbon isotope fractionation (εC = -2.0‰). Hence dual element isotope analysis bears potential not only to detect diclofenac degradation, but even to distinguish both transformation pathways in the environment. In an explorative survey, analysis of commercial diclofenac products showed significant differences in carbon and nitrogen isotope ratios, demonstrating a further potential to track, and potentially even to authenticate, commercial production batches.
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Publication type
Article: Journal article
Document type
Scientific Article
Keywords
Pharmaceutical Residues; Acidic Pharmaceuticals; Mass-spectrometry; Drug Diclofenac; Waste-water; Fractionation; Biodegradation; Degradation; Pathways; River
ISSN (print) / ISBN
0013-936X
e-ISSN
1520-5851
Quellenangaben
Volume: 48,
Issue: 4,
Pages: 2312-2320
Publisher
American Chemical Society (ACS)
Publishing Place
Washington, DC
Reviewing status
Peer reviewed
Institute(s)
Institute of Groundwater Ecology (IGOE)