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C & N isotope analysis of diclofenac to distinguish oxidative and reductive transformation and to track commercial products

Michael P Maier, Simon De Corte UGent, Sebastian Nitsche, Thomas Spaett, Nico Boon UGent and Martin Elsner (2014) ENVIRONMENTAL SCIENCE & TECHNOLOGY. 48(4). p.2312-2320
abstract
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-mu gL(-1) range in environmental samples. Degradation in an aerobic sediment-water system showed strong nitrogen isotope fractionation (epsilon(N) = -7.1 parts per thousand), whereas reductive diclofenac dechlorination was associated with significant carbon isotope fractionation (epsilon(C) = -2.0 parts per thousand). 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.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
subject
keyword
MASS-SPECTROMETRY, ACIDIC PHARMACEUTICALS, DRUG DICLOFENAC, WASTE-WATER, FRACTIONATION, BIODEGRADATION, DEGRADATION, PATHWAYS, RIVER, PHARMACEUTICAL RESIDUES
journal title
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Environ. Sci. Technol.
volume
48
issue
4
pages
2312 - 2320
Web of Science type
Article
Web of Science id
000331774100027
JCR category
ENVIRONMENTAL SCIENCES
JCR impact factor
5.33 (2014)
JCR rank
10/223 (2014)
JCR quartile
1 (2014)
ISSN
0013-936X
DOI
10.1021/es403214z
language
English
UGent publication?
yes
classification
A1
copyright statement
I have transferred the copyright for this publication to the publisher
id
4345453
handle
http://hdl.handle.net/1854/LU-4345453
date created
2014-03-27 16:13:24
date last changed
2016-12-19 15:43:43
@article{4345453,
  abstract     = {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-mu gL(-1) range in environmental samples. Degradation in an aerobic sediment-water system showed strong nitrogen isotope fractionation (epsilon(N) = -7.1 parts per thousand), whereas reductive diclofenac dechlorination was associated with significant carbon isotope fractionation (epsilon(C) = -2.0 parts per thousand). 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.},
  author       = {Maier, Michael P and De Corte, Simon and Nitsche, Sebastian and Spaett, Thomas and Boon, Nico and Elsner, Martin},
  issn         = {0013-936X},
  journal      = {ENVIRONMENTAL SCIENCE \& TECHNOLOGY},
  keyword      = {MASS-SPECTROMETRY,ACIDIC PHARMACEUTICALS,DRUG DICLOFENAC,WASTE-WATER,FRACTIONATION,BIODEGRADATION,DEGRADATION,PATHWAYS,RIVER,PHARMACEUTICAL RESIDUES},
  language     = {eng},
  number       = {4},
  pages        = {2312--2320},
  title        = {C \& N isotope analysis of diclofenac to distinguish oxidative and reductive transformation and to track commercial products},
  url          = {http://dx.doi.org/10.1021/es403214z},
  volume       = {48},
  year         = {2014},
}

Chicago
Maier, Michael P, Simon De Corte, Sebastian Nitsche, Thomas Spaett, Nico Boon, and Martin Elsner. 2014. “C & N Isotope Analysis of Diclofenac to Distinguish Oxidative and Reductive Transformation and to Track Commercial Products.” Environmental Science & Technology 48 (4): 2312–2320.
APA
Maier, M. P., De Corte, S., Nitsche, S., Spaett, T., Boon, N., & Elsner, M. (2014). C & N isotope analysis of diclofenac to distinguish oxidative and reductive transformation and to track commercial products. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 48(4), 2312–2320.
Vancouver
1.
Maier MP, De Corte S, Nitsche S, Spaett T, Boon N, Elsner M. C & N isotope analysis of diclofenac to distinguish oxidative and reductive transformation and to track commercial products. ENVIRONMENTAL SCIENCE & TECHNOLOGY. 2014;48(4):2312–20.
MLA
Maier, Michael P, Simon De Corte, Sebastian Nitsche, et al. “C & N Isotope Analysis of Diclofenac to Distinguish Oxidative and Reductive Transformation and to Track Commercial Products.” ENVIRONMENTAL SCIENCE & TECHNOLOGY 48.4 (2014): 2312–2320. Print.