Microbial in situ degradation of aromatic hydrocarbons in a contaminated aquifer monitored by carbon isotope fractionation

Richnow, Hans H.; Annweiler, Eva; Michaelis, Walter; Meckenstock, Rainer U.

doi:10.1016/s0169-7722(02)00233-4

Cited by 140 publications

(119 citation statements)

References 24 publications

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“…The general feasibility of such an approach has been demonstrated in a number of studies (71,(97)(98)(99)(100)(101)(102)(103) and is discussed in a comprehensive recent review by Meckenstock et al (24). Here we focus primarily on the aspect how insight about transformation pathways can aid in choosing the appropriate isotopic enrichment factor ( bulk) that is needed to quantify the extent of in situ transformation according to eq 8.…”

Section: Consequences For the Assessment Of Isotope Fractionation In mentioning

confidence: 99%

A New Concept Linking Observable Stable Isotope Fractionation to Transformation Pathways of Organic Pollutants

Elsner

Zwank

Hunkeler

et al. 2005

Environ. Sci. Technol.

502

803

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Measuring stable isotope fractionation of carbon, hydrogen, and other elements by Compound Specific Isotope Analysis (CSIA) is a new, innovative approach to assess organic pollutant degradation in the environment. Central to this concept is the Rayleigh equation which relates degradation-induced decreases in concentrations directly to concomitant changes in bulk () average over the whole compound) isotope ratios. The extent of in situ transformation may therefore be inferred from measured isotope ratios in field samples, provided that an appropriate enrichment factor ( bulk ) is known. This bulk value, however, is usually only valid for a specific compound and for specific degradation conditions. Therefore, a direct comparison of bulk values for different compounds and for different types of reactions has in general not been feasible. In addition, it is often uncertain how robust and reproducible bulk values are and how confidently they can be used to quantify contaminant degradation in the field. To improve this situation and to achieve a more in-depth understanding, this critical review aims to relate fundamental insight about kinetic isotope effects (KIE) found in the physico(bio)chemical literature to apparent kinetic isotope effects (AKIE) derived from bulk values reported in environmentally oriented studies. Starting from basic rate laws, a quite general derivation of the Rayleigh equation is given, resulting in a novel set of simple equations that take into account the effects of (1) nonreacting positions and (2) intramolecular competition and that lead to position-specific AKIE values rather than bulk enrichment factors. Reevaluation of existing bulk literature values result in consistent ranges of AKIE values that generally are in good agreement with previously published data in the (bio)-chemical literature and are typical of certain degradation reactions (subscripts C and H indicate values for carbon and hydrogen): AKIE C ) 1.01-1.03 and AKIE H ) 2-23 for oxidation of C-H bonds; AKIE C ) 1.03-1.07 for S N 2-

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Section: Consequences For the Assessment Of Isotope Fractionation In mentioning

confidence: 99%

A New Concept Linking Observable Stable Isotope Fractionation to Transformation Pathways of Organic Pollutants

Elsner

Zwank

Hunkeler

et al. 2005

Environ. Sci. Technol.

502

803

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“…Although the Rayleigh equation was originally developed for homogeneous batch systems (18), it is increasingly applied for flow-through systems such as column and field studies (1)(2)(3)(4)(5)(6)(7)(8)(9)(11)(12)(13)(14)(15). In a flow through system, physical and chemical heterogeneity influences the interpretation of isotope data and is expected to lead to an underestimation of the amount of biodegradation when the Rayleigh equation is applied, as recently shown by Kopinke et al 2005 (17).…”

Section: Introductionmentioning

confidence: 99%

Does the Rayleigh Equation Apply to Evaluate Field Isotope Data in Contaminant Hydrogeology?

Abe

Hunkeler

2006

Environ. Sci. Technol.

125

119

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Stable isotope data have been increasingly used to assess in situ biodegradation of organic contaminants in groundwater. The data are usually evaluated using the Rayleigh equation to evaluate whether isotope data follow a Rayleigh trend, to calculate the extent of contaminant biodegradation, or to estimate first-order rate constants. However, the Rayleigh equation was developed for homogeneous systems while in the subsurface, contaminants can migrate at different velocities due to physical heterogeneity. This paper presents a method to quantify the systematic effect that is introduced by applying the Rayleigh equation to field isotope data. For this purpose, the travel time distribution between source and sampling point is characterized by an analytical solution to the advection-dispersion equation. The systematic effect was evaluated as a function of the magnitude of physical heterogeneity, geometry of the contaminant plume, and degree of biodegradation. Results revealed that the systematic effect always leads to an underestimation of the actual values of isotope enrichment factors, the extent of biodegradation, or first-order rate constants, especially in the dispersion-dominant region representing a higher degree of physical heterogeneity. A substantial systematic effect occurs especially for the quantification of firstorder rate constants (up to 50% underestimation of actual rate) while it is relatively small for quantification of the extent of biodegradation (<5% underestimation of actual degree of biodegradation). The magnitude of the systematic effect is in the same range as the uncertainty due to uncertainty of the analytical data, of the isotope enrichment factor, and the average travel time.

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“…Isotope compositions of PCDDs and chloroethenes was by gas chromatography-combustionisotope ratio mass spectrometry (GC-C-IRMS) using an Agilent 6890 GC (Agilent Technologies, Inc. Santa Clara, CA) connected to a Finnigan MAT 252 mass spectrometer via a Finnigan GC-C/TC III Interface (Richnow et al, 2003;Nijenhuis et al, 2007;Cichocka et al, 2008). PCDDs were separated on a ZB-5 column (60 m × 0.32 mm I.D.…”

Section: Methodsmentioning

confidence: 99%

“…CSIA detects fractionation resulting from the kinetic isotope effect (KIE) caused by different reaction rates for a compound containing the heavy isotope versus the light isotope at the location of the reaction, and from other environmental processes (Schmidt et al, 2004). CSIA was examined for fuel components (Meckenstock, 1999;Hunkeler et al, 2001;Gray et al, 2002;Somsamak et al, 2005); aromatic hydrocarbons (Richnow et al, 2003;Yanik et al, 2003;Hall et al, 1999); and halogenated compounds (Hunkeler et al, 1999;Bloom et al, 2000;Sherwood Lollar et al, 2001;Drenzek et al, 2001;Nijenhuis et al, 2005;, Cichocka et al, 2008. CSIA could be useful for monitoring fate of the polychlorinated dibenzo-p-dioxins (PCDDs).…”

Section: Introductionmentioning

confidence: 99%

Quantifying Enhanced Microbial Dehalogenation Impacting the Fate and Transport of Organohalide Mixtures in Contaminated Sediments

Häggblom¹,

Fennell²,

Rodenburg³

et al. 2012

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Standard Form 298 (Rev. 8/98) REPORT DOCUMENTATION PAGEPrescribed by ANSI Std. Z39.18 Form Approved OMB No. 0704-0188The public reporting burden for this collection of information is estimated to average 1 hour per response, including the time for reviewing instructions, searching existing data sources, gathering and maintaining the data needed, and completing and reviewing the collection of information. Send comments regarding this burden estimate or any other aspect of this collection of information, including suggestions for reducing the burden, to the Department of Defense, Executive Services and Communications Directorate (0704-0188). Respondents should be aware that notwithstanding any other provision of law, no person shall be subject to any penalty for failing to comply with a collection of information if it does not display a currently valid OMB control number. PLEASE DO NOT RETURN YOUR FORM TO THE ABOVE ORGANIZATION. 1. REPORT DATE (DD-MM-YYYY)2. REPORT TYPE 3. DATES COVERED (From -To) 4. TITLE AND SUBTITLE 5a. CONTRACT NUMBER 5b. GRANT NUMBER 5c. PROGRAM ELEMENT NUMBER 5d. PROJECT NUMBER 5e. TASK NUMBER 5f. WORK UNIT NUMBER AUTHOR(S) PERFORMING ORGANIZATION NAME(S) AND ADDRESS(ES) 8. PERFORMING ORGANIZATION REPORT NUMBER SPONSORING/MONITORING AGENCY NAME(S) AND ADDRESS(ES) 10. SPONSOR/MONITOR'S ACRONYM(S) SPONSOR/MONITOR'S REPORT NUMBER(S)12 SERDPThe project investigated techniques and amendments to enhance microbial dehalogenation in sediments contaminated with organohalide mixtures and developed methods and tools to monitor the effectiveness of biostimulation processes. Micro-and mesocosm studies with organohalide-contaminated sediments demonstrated that these contain diverse communities of dehalogenating microorganisms. Dechlorination of historical PCB and PCDD/F contaminant mixtures can be stimulated by addition of amendments and/or bioaugmentation with dechlorinating bacteria. The enhanced dechlorination correlates with increased numbers of dehalorespirer populations and reductive dehalogenase genes. Identification of the specific microbial members associated with PCB-and PCDD/F-dechlorinating activity should allow for better strategies to enhance dehalogenation. The results provide compelling evidence to support further testing and development of biostimulation and bioaugmentation with dehalorespiring bacteria as environmentally less invasive and lower cost alternatives for in situ treatment of PCB impacted sediments. Anacostia microcosms compared to the sum of all di-through deca-chlorinated biphenyls (homolog groups 2 through 10). Analyses of the dry matter content, the total PCB concentration, the average number and percentage of chlorines less than 4 and 6, respectively and in soil samples and commercial Aroclor mixtures. Table 6-2. Analyses of total bacteria, putative dechlorinating and PCB degrading bacteria and the number of dechlorinating bacteria in soil samples. Table 6-3. The potential dechlorination activi...

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Microbial in situ degradation of aromatic hydrocarbons in a contaminated aquifer monitored by carbon isotope fractionation

Cited by 140 publications

References 24 publications

A New Concept Linking Observable Stable Isotope Fractionation to Transformation Pathways of Organic Pollutants

A New Concept Linking Observable Stable Isotope Fractionation to Transformation Pathways of Organic Pollutants

Does the Rayleigh Equation Apply to Evaluate Field Isotope Data in Contaminant Hydrogeology?

Quantifying Enhanced Microbial Dehalogenation Impacting the Fate and Transport of Organohalide Mixtures in Contaminated Sediments

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