Project

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Assessing Sources and Fate of Marine Natural Halogenated Phenolic Compounds Using Their Stable Halogen Isotopes

English title Assessing Sources and Fate of Marine Natural Halogenated Phenolic Compounds Using Their Stable Halogen Isotopes
Applicant Aeppli Christoph
Number 134124
Funding scheme Fellowships for advanced researchers
Research institution Dept. of Marine Chemistry and Geochemistry Woods Hole Oceanographic Institution
Institution of higher education Institution abroad - IACH
Main discipline Other disciplines of Environmental Sciences
Start/End 01.05.2011 - 30.04.2013
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All Disciplines (2)

Discipline
Other disciplines of Environmental Sciences
Geochemistry

Keywords (8)

marine coastal environments; stable isotopes; oil spill; Deepwater Horizon; photooxidation; biodegradation; organic pollutants; natural halogenated compounds

Lay Summary (English)

Lead
Lay summary

Marine coastal environments are under stress from anthropogenic activities, and organic pollutants are of great concern. This project targets two aspects of organic contaminants in marine coastal environments: natural formation of organohalogens, and degradation processes of oil compounds.

In the first part of this project, brominated phenolic compounds, which are often associated with toxic effects, are investigated. Recently, a variety of such compounds that have a natural origin have been detected in seawater, sediments, and along the marine food chain. Since these compounds are also industrially produced, apportion natural and anthropogenic sources is important for global emission budgets. The aim of this project is to make use of isotopic ‘fingerprints’, which are expected to be different for naturally and industrially produced halogenated compounds, for such a source apportionment. Furthermore, isotopic analysis is expected to provide new insights into natural halogenation pathways used by marine algae and worms. The proposed project is expected to highlight the potential of isotope-based apportionment of natural and anthropogenic halogenated compounds in marine systems.

The second part of this project is to investigate oil weathering processes after offshore oil spills. Specifically, the long-term fate of weathered oil in coastal environment will be studied. Furthermore, the compositional changes of the spilled oil upon biodegradation and photooxidation will be analyzed. Thereby, especially polar compounds with toxic properties, which have been suggested to be formed upon oil weathering, will be targeted. Samples collected on sea surface and on beaches in the Gulf of Mexico immediately after and up to 18 month after the Deepwater Horizon oil spill will be analyzed using a variety of analytical techniques to study molecular and bulk properties and isotopic composition of non-polar as well as of polar fractions of weathered oil. The project is expected to lead to new insights about long term impact of oil spills on marine coastal environments.

Direct link to Lay Summary Last update: 21.02.2013

Responsible applicant and co-applicants

Publications

Publication
Use of Cl and C Isotopic Fractionation to Identify Degradation and Sources of Polychlorinated Phenols: Mechanistic Study and Field Application
Aeppli Christoph, Tysklind Mats, Holmstrand Henry, Gustafsson Orjan (2013), Use of Cl and C Isotopic Fractionation to Identify Degradation and Sources of Polychlorinated Phenols: Mechanistic Study and Field Application, in ENVIRONMENTAL SCIENCE & TECHNOLOGY, 47(2), 790-797.
Dual Carbon-Chlorine Stable Isotope Investigation of Sources and Fate of Chlorinated Ethenes in Contaminated Groundwater
Wiegert Charline, Aeppli Christoph, Knowles Tim, Holmstrand Henry, Evershed Richard, Pancost Richard D., Machackova Jirina, Gustafsson Orjan (2012), Dual Carbon-Chlorine Stable Isotope Investigation of Sources and Fate of Chlorinated Ethenes in Contaminated Groundwater, in ENVIRONMENTAL SCIENCE & TECHNOLOGY, 46(20), 10918-10925.
Oil Weathering after the Deepwater Horizon Disaster Led to the Formation of Oxygenated Residues
Aeppli Christoph, Carmichael Catherine A., Nelson Robert K., Lemkau Karin L., Graham William M., Redmond Molly C., Valentine David L., Reddy Christopher M. (2012), Oil Weathering after the Deepwater Horizon Disaster Led to the Formation of Oxygenated Residues, in ENVIRONMENTAL SCIENCE & TECHNOLOGY, 46(16), 8799-8807.
Carbon and Chlorine Isotope Fractionation During Microbial Degradation of Tetra- and Trichloroethene
Wiegert C., Mandalakis M., Knowles T., Polymenakou P.N., Aeppli C., Machackova J., Holmstrand H., Evershed R.P., Pancost R.D., Gustafsson O., Carbon and Chlorine Isotope Fractionation During Microbial Degradation of Tetra- and Trichloroethene, in Environmental Science and Technology, doi:10.102.
Chlorine isotope effects and composition of naturally produced organochlorines from chloroperoxidases, flavin-dependent halogenases, and in forest soil
Aeppli C., Bastviken D., Andersson P., Gustafsson Ö., Chlorine isotope effects and composition of naturally produced organochlorines from chloroperoxidases, flavin-dependent halogenases, and in forest soil, in Environmental Science and Technology, doi:10.102.

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
SETAC North America 32th annual meeting 13.11.2011 Boston, MA, USA
ACS Meeting Denve 28.08.2011 Denver, CO, USA


Abstract

Natural halogenated compounds (NHCs) are prevalent in marine environment, and a variety of phenolic NHCs have been detected in seawater, sediments, and along the marine food chain. Since many NHCs have also industrially produced analogs, apportion natural and anthropogenic sources is important for global emission budgets, which are often lacking data of NHC production. Beside formation, also NHC degradation is of importance, since the same reaction pathways that nature uses for dehalogenating NHCs are also used for biodegrading a variety of anthropogenic halogenated pollutants. The aim of this project is to assess marine phenolic NHC formation and degradation using compound-specific isotope analysis. While the use of stable halogen and carbon isotopes are very powerful to assess the formation and degradation of NHCs, radiocarbon analysis (C-14) allows for apportion natural and industrial sources of halogenated compounds. The objectives of the proposed research are to characterize kinetic isotope effects associated with phenolic NHC production as well as degradation in well-defined laboratory systems. This information will then be used for isotope-based identification of NHCs formation pathways in marine algae and worms, as well as for assessment of NHC dynamics in marine costal and open ocean systems.Novel continuous-flow analytical methods for analyzing chlorine, bromine, and carbon stable isotopes (based on GC/MS, GC/ICP/MS, and GC/C/IRMS) will be used for analysis of the target phenolic NHCs. Radiocarbon analysis will be preformed for source apportionment for selected analytes using accelerated mass spectrometry (AMS). Experiments will be conducted with pure enzymes as well as with crude extracts of algal and worm enzymes, and NHCs will be analyzed from marine biota, seawater and sediments.The proposed project is expected to allow isotope-based apportionment of natural and anthropogenic halogenated compounds in marine systems of different spatial scales (benthic biota, costal environment, and open ocean). Furthermore, it will provide insights on a molecular level in halogenation mechanisms of marine organisms, as well as in NHC dechlorination pathways.
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