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Application of two dimensional compound specific carbon-chlorine isotope analyses for degradation monitoring and assessment of organic pollutants in contaminated soil and groundwater
Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
2013 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Nearly 250,000 sites with past and present potentially polluting activities need urgent remediation within Europe. Major pollutants include organochlorines (OCls), e.g. chlorinated ethenes (CEs) and hexachlorocyclohexanes (HCHs), mainly used as industrial solvents and pesticides, respectively. Due to improper handling and disposal, OCls contaminants are present in the soil or groundwater surrounding sites, where they have been produced or used. CEs and HCHs can undergo degradation by microorganisms indigenous to the soil or groundwater. Therefore natural attenuation (NA), relying on the in situ biodegradation of pollutants, is considered as a cost effective remediation strategy, yet it requires accurate monitoring methods. Compound specific isotope analysis (CSIA) is a powerful tool to provide information on the extent of degradation and, when combining two isotope systems (2D-CSIA), such as carbon (δ13C) and chlorine (δ37Cl), on reaction mechanisms.

The diagnostic reaction-specific isotope enrichment factors (εC and εCl) were determined in laboratory experiments for the anaerobic degradation of PCE, TCE (Paper II) and α-HCH (Paper III) by mixed bacterial cultures enriched from CEs and HCHs contaminated sites, respectively. The related mechanism-specific εClC ratios were calculated as 0.35 ± 0.11 (PCE), 0.37 ± 0.11 (TCE) and 0.52 ± 0.23 (α-HCH). These values are smaller than previously reported values for pure cultures. This is explained by the microbial community composition changes observed during degradation of PCE and α-HCH, which also reflect the variability of the microbial community at the field level. Furthermore, εClC ratio might be bacteria specific.

These values allowed the estimation of the extent of contaminant degradation at the respective study sites (Paper III and IV). Application of both isotope systems (δ13C and δ37Cl) led to comparable estimates. However the choice of representative ε values is crucial for an accurate assessment.

These studies show that CSIA is useful to quantify in situ degradation of OCls contaminants and identify reaction pathways, by combining δ13C and δ37Cl.

Place, publisher, year, edition, pages
Stockholm: Department of Applied Environmental Science (ITM), Stockholm University , 2013. , 52 p.
Keyword [en]
organochlorines, chlorinated ethenes, PCE, TCE, hexachlorocyclohexanes, soil contamination, groundwater contamination, remediation, natural attenuation, biodegradation, carbon isotopes, chlorine isotopes, CSIA
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
URN: urn:nbn:se:su:diva-93923ISBN: 978-91-7447-762-7 (print)OAI: oai:DiVA.org:su-93923DiVA: diva2:650032
Public defence
2013-11-01, Nordenskiöldsalen, Geovetenskapens hus, Svante Arrhenius väg 12, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 3: Submitted. Paper 4: Manuscript.

Available from: 2013-10-10 Created: 2013-09-19 Last updated: 2013-10-04Bibliographically approved
List of papers
1. Dual carbon chlorine stable isotope investigation of sources and fate of chlorinated ethenes in contaminated groundwater
Open this publication in new window or tab >>Dual carbon chlorine stable isotope investigation of sources and fate of chlorinated ethenes in contaminated groundwater
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2012 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 46, no 20, 10918-10925 p.Article in journal (Refereed) Published
Abstract [en]

Chlorinated ethenes (CEs) are ubiquitous groundwater contaminants, yet there remains a need for a method to efficiently monitor their in situ degradation. We report here the first field application of combined stable carbon and chlorine isotope analysis of tetrachloroethene (PCE) and trichloroethene (TCE) to investigate their biodegradation in a heavily contaminated aquifer. The two-dimensional Compound Specific Isotope Analysis (2D-CSIA) approach was facilitated by a recently developed gas chromatography-quadrupole mass spectrometry (GCqMS) method for delta Cl-37 determination. Both C and Cl isotopes showed evidence of ongoing PCE transformation. Applying published C isotope enrichment factors (epsilon(C)) enabled evaluation of the extent of in situ PCE degradation (11-78%). We interpreted C and Cl isotopes using a numerical reactive transport model along a 60-m flow path. It revealed that combined PCE and TCE mass load was dechlorinated by less than 10%, and that cis-dichloroethene was not further dechlorinated. Furthermore, the 2D-CSIA approach allowed estimation of Cl isotope enrichment factors epsilon(Cl) (-7.8 to -0.8 parts per thousand) and characteristic epsilon(Cl)/epsilon(C) values (0.42-1.12) for reductive PCE dechlorination at this field site. This investigation demonstrates the benefit of 2D-CSIA to assess in situ degradation of CEs and the applicability of Cl isotope fractionation to evaluate PCE and TCE dechlorination.

National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-83964 (URN)10.1021/es3016843 (DOI)000309805000011 ()
Note

AuthorCount:8;

Available from: 2012-12-18 Created: 2012-12-17 Last updated: 2017-12-06Bibliographically approved
2. Carbon and Chlorine Isotope Fractionation During Microbial Degradation of Tetra- and Trichloroethene
Open this publication in new window or tab >>Carbon and Chlorine Isotope Fractionation During Microbial Degradation of Tetra- and Trichloroethene
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2013 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 47, no 12, 6449-6456 p.Article in journal (Refereed) Published
Abstract [en]

Two-dimensional compound-specific isotope analysis (2D-CSIA), combining stable carbon and chlorine isotopes, holds potential for monitoring of natural attenuation of chlorinated ethenes (CEs), in contaminated soil and groundwater. However, interpretation of 2D-CSIA data sets is challenged by a shortage of experimental Cl isotope enrichment factors. Here, isotope enrichments factors for C and Cl (i.e., epsilon(C) and epsilon(Cl)) were determined for biodegradation of tetrachloroethene (PCE) and trichloroethene (TCE) using microbial enrichment cultures from a heavily CE-contaminated aquifer. The obtained values were epsilon(C) = -5.6 +/- 0.7 parts per thousand (95% CI) and epsilon(Cl) = -2.0 +/- 0.5 parts per thousand for PCE degradation and epsilon(C) = -8.8 +/- 0.2 parts per thousand and epsilon(Cl) = -3.5 +/- 0.5 parts per thousand for TCE degradation. Combining the values for both epsilon(C) and epsilon(Cl) yielded mechanism-diagnostic epsilon(Cl)/epsilon(C) ratios of 0.35 +/- 0.11 and 0.37 +/- 0.11 degradation of PCE and TCE, respectively. Application of the obtained epsilon(C) and epsilon(Cl) values to a previously investigated field site gave similar estimates for the fraction of degraded contaminant as in the previous study, but with a reduced uncertainty in assessment of the natural attenuation. Furthermore, 16S rRNA gene clone library analyses were performed on three samples from the PCE degradation experiments. A species closely related to Desulfitobacterium aromaticivorans UKTL dominated the reductive dechlorination process. This study contributes to the development of 2D-CSIA as a tool for evaluating remediation strategies of CEs at contaminated sites.

National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-92812 (URN)10.1021/es305236y (DOI)000320749000047 ()
Note

AuthorCount:10;

Available from: 2013-08-22 Created: 2013-08-20 Last updated: 2017-12-06Bibliographically approved
3. Carbon and Chlorine Stable Isotope Fractionation during Anaerobic Degradation of α-Hexachlorocyclohexane by a Mixed Culture Enriched from a Contaminated Site
Open this publication in new window or tab >>Carbon and Chlorine Stable Isotope Fractionation during Anaerobic Degradation of α-Hexachlorocyclohexane by a Mixed Culture Enriched from a Contaminated Site
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(English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851Article in journal (Refereed) Submitted
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-93920 (URN)
Available from: 2013-09-19 Created: 2013-09-19 Last updated: 2017-12-06Bibliographically approved
4. Carbon Stable Isotope Investigation of Hexachlorocyclohexanes in Field Contaminated Soils
Open this publication in new window or tab >>Carbon Stable Isotope Investigation of Hexachlorocyclohexanes in Field Contaminated Soils
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(English)Manuscript (preprint) (Other academic)
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-93922 (URN)
Available from: 2013-09-19 Created: 2013-09-19 Last updated: 2013-09-25Bibliographically approved

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