Fate of triclosan and evidence for reductive dechlorination of triclocarban in estuarine sediments

Todd R. Miller, Jochen Heidler, Steven N. Chillrud, Amelia Delaquil, Jerry C. Ritchie, Jana N. Mihalic, Richard Bopp, Rolf Halden

Research output: Contribution to journalArticle

151 Citations (Scopus)

Abstract

The biocides triclosan and triclocarban are wastewater contaminants whose occurrence and fate in estuarine sediments remain unexplored. We examined contaminant profiles in 137Cs/7Be-dated sediment cores taken near wastewater treatment plants in the Chesapeake Bay watershed (CB), Maryland and Jamaica Bay (JB), New York. In JB, biocide occurrences tracked the time course of biocide usage and wastewater treatment strategies employed, first appearing in the 1950s (triclocarban) and 1960s (triclosan), and peaking in the late 1960s and 1970s (24 ± 0.54 and 0.8 ± 0.4 mg/kg dry weight, respectively). In CB, where the time of sediment accumulation was not as well constrained by 137Cs depth profiles, triclocarban was only measurable in 137Cs-bearing sediments, peaking at 3.6 ± 0.6 mg/kg midway through the core and exceeding 1 mg/kg in recent deposits. In contrast, triclosan concentrations were low or not detectable in the CB core. Analysis of CB sediment by tandem mass spectrometry produced the first evidence for complete sequential dechlorination of triclocarban to the transformation products dichloro-, monochloro-, and unsubstituted carbanilide, which were detected at maxima of 15.5 ± 1.8, 4.1 ± 2.4, and 0.5 ± 0.1 mg/kg, respectively. Concentrations of all carbanilide congeners combined were correlated with heavy metals [R2 > 0.64, P < 0.01), thereby identifying wastewater as the principal pathway of contamination, Environmental persistence over the past 40 years was observed for triclosan and triclocarban in JB, and for triclocarban's diphenylurea backbone in CB sediments.

Original languageEnglish (US)
Pages (from-to)4570-4576
Number of pages7
JournalEnvironmental Science and Technology
Volume42
Issue number12
DOIs
StatePublished - Jun 15 2008

Fingerprint

Triclosan
Dechlorination
estuarine sediment
dechlorination
Watersheds
Sediments
Carbanilides
Biocides
Disinfectants
watershed
Wastewater treatment
pesticide
Wastewater
Bearings (structural)
Impurities
sediment
Heavy Metals
wastewater
Heavy metals
Mass spectrometry

ASJC Scopus subject areas

  • Environmental Engineering
  • Environmental Science(all)
  • Environmental Chemistry

Cite this

Fate of triclosan and evidence for reductive dechlorination of triclocarban in estuarine sediments. / Miller, Todd R.; Heidler, Jochen; Chillrud, Steven N.; Delaquil, Amelia; Ritchie, Jerry C.; Mihalic, Jana N.; Bopp, Richard; Halden, Rolf.

In: Environmental Science and Technology, Vol. 42, No. 12, 15.06.2008, p. 4570-4576.

Research output: Contribution to journalArticle

Miller, TR, Heidler, J, Chillrud, SN, Delaquil, A, Ritchie, JC, Mihalic, JN, Bopp, R & Halden, R 2008, 'Fate of triclosan and evidence for reductive dechlorination of triclocarban in estuarine sediments', Environmental Science and Technology, vol. 42, no. 12, pp. 4570-4576. https://doi.org/10.1021/es702882g
Miller, Todd R. ; Heidler, Jochen ; Chillrud, Steven N. ; Delaquil, Amelia ; Ritchie, Jerry C. ; Mihalic, Jana N. ; Bopp, Richard ; Halden, Rolf. / Fate of triclosan and evidence for reductive dechlorination of triclocarban in estuarine sediments. In: Environmental Science and Technology. 2008 ; Vol. 42, No. 12. pp. 4570-4576.
@article{f05937e65dcb4d0c843cd3f2eff25062,
title = "Fate of triclosan and evidence for reductive dechlorination of triclocarban in estuarine sediments",
abstract = "The biocides triclosan and triclocarban are wastewater contaminants whose occurrence and fate in estuarine sediments remain unexplored. We examined contaminant profiles in 137Cs/7Be-dated sediment cores taken near wastewater treatment plants in the Chesapeake Bay watershed (CB), Maryland and Jamaica Bay (JB), New York. In JB, biocide occurrences tracked the time course of biocide usage and wastewater treatment strategies employed, first appearing in the 1950s (triclocarban) and 1960s (triclosan), and peaking in the late 1960s and 1970s (24 ± 0.54 and 0.8 ± 0.4 mg/kg dry weight, respectively). In CB, where the time of sediment accumulation was not as well constrained by 137Cs depth profiles, triclocarban was only measurable in 137Cs-bearing sediments, peaking at 3.6 ± 0.6 mg/kg midway through the core and exceeding 1 mg/kg in recent deposits. In contrast, triclosan concentrations were low or not detectable in the CB core. Analysis of CB sediment by tandem mass spectrometry produced the first evidence for complete sequential dechlorination of triclocarban to the transformation products dichloro-, monochloro-, and unsubstituted carbanilide, which were detected at maxima of 15.5 ± 1.8, 4.1 ± 2.4, and 0.5 ± 0.1 mg/kg, respectively. Concentrations of all carbanilide congeners combined were correlated with heavy metals [R2 > 0.64, P < 0.01), thereby identifying wastewater as the principal pathway of contamination, Environmental persistence over the past 40 years was observed for triclosan and triclocarban in JB, and for triclocarban's diphenylurea backbone in CB sediments.",
author = "Miller, {Todd R.} and Jochen Heidler and Chillrud, {Steven N.} and Amelia Delaquil and Ritchie, {Jerry C.} and Mihalic, {Jana N.} and Richard Bopp and Rolf Halden",
year = "2008",
month = "6",
day = "15",
doi = "10.1021/es702882g",
language = "English (US)",
volume = "42",
pages = "4570--4576",
journal = "Environmental Science & Technology",
issn = "0013-936X",
publisher = "American Chemical Society",
number = "12",

}

TY - JOUR

T1 - Fate of triclosan and evidence for reductive dechlorination of triclocarban in estuarine sediments

AU - Miller, Todd R.

AU - Heidler, Jochen

AU - Chillrud, Steven N.

AU - Delaquil, Amelia

AU - Ritchie, Jerry C.

AU - Mihalic, Jana N.

AU - Bopp, Richard

AU - Halden, Rolf

PY - 2008/6/15

Y1 - 2008/6/15

N2 - The biocides triclosan and triclocarban are wastewater contaminants whose occurrence and fate in estuarine sediments remain unexplored. We examined contaminant profiles in 137Cs/7Be-dated sediment cores taken near wastewater treatment plants in the Chesapeake Bay watershed (CB), Maryland and Jamaica Bay (JB), New York. In JB, biocide occurrences tracked the time course of biocide usage and wastewater treatment strategies employed, first appearing in the 1950s (triclocarban) and 1960s (triclosan), and peaking in the late 1960s and 1970s (24 ± 0.54 and 0.8 ± 0.4 mg/kg dry weight, respectively). In CB, where the time of sediment accumulation was not as well constrained by 137Cs depth profiles, triclocarban was only measurable in 137Cs-bearing sediments, peaking at 3.6 ± 0.6 mg/kg midway through the core and exceeding 1 mg/kg in recent deposits. In contrast, triclosan concentrations were low or not detectable in the CB core. Analysis of CB sediment by tandem mass spectrometry produced the first evidence for complete sequential dechlorination of triclocarban to the transformation products dichloro-, monochloro-, and unsubstituted carbanilide, which were detected at maxima of 15.5 ± 1.8, 4.1 ± 2.4, and 0.5 ± 0.1 mg/kg, respectively. Concentrations of all carbanilide congeners combined were correlated with heavy metals [R2 > 0.64, P < 0.01), thereby identifying wastewater as the principal pathway of contamination, Environmental persistence over the past 40 years was observed for triclosan and triclocarban in JB, and for triclocarban's diphenylurea backbone in CB sediments.

AB - The biocides triclosan and triclocarban are wastewater contaminants whose occurrence and fate in estuarine sediments remain unexplored. We examined contaminant profiles in 137Cs/7Be-dated sediment cores taken near wastewater treatment plants in the Chesapeake Bay watershed (CB), Maryland and Jamaica Bay (JB), New York. In JB, biocide occurrences tracked the time course of biocide usage and wastewater treatment strategies employed, first appearing in the 1950s (triclocarban) and 1960s (triclosan), and peaking in the late 1960s and 1970s (24 ± 0.54 and 0.8 ± 0.4 mg/kg dry weight, respectively). In CB, where the time of sediment accumulation was not as well constrained by 137Cs depth profiles, triclocarban was only measurable in 137Cs-bearing sediments, peaking at 3.6 ± 0.6 mg/kg midway through the core and exceeding 1 mg/kg in recent deposits. In contrast, triclosan concentrations were low or not detectable in the CB core. Analysis of CB sediment by tandem mass spectrometry produced the first evidence for complete sequential dechlorination of triclocarban to the transformation products dichloro-, monochloro-, and unsubstituted carbanilide, which were detected at maxima of 15.5 ± 1.8, 4.1 ± 2.4, and 0.5 ± 0.1 mg/kg, respectively. Concentrations of all carbanilide congeners combined were correlated with heavy metals [R2 > 0.64, P < 0.01), thereby identifying wastewater as the principal pathway of contamination, Environmental persistence over the past 40 years was observed for triclosan and triclocarban in JB, and for triclocarban's diphenylurea backbone in CB sediments.

UR - http://www.scopus.com/inward/record.url?scp=45249084784&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=45249084784&partnerID=8YFLogxK

U2 - 10.1021/es702882g

DO - 10.1021/es702882g

M3 - Article

VL - 42

SP - 4570

EP - 4576

JO - Environmental Science & Technology

JF - Environmental Science & Technology

SN - 0013-936X

IS - 12

ER -