Compound-specific stable isotope analysis of organic contaminants in natural environments: a critical review of the state of the art,prospects, and future challenges |
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Authors: | Email author" target="_blank">Torsten?C?SchmidtEmail author Luc?Zwank Martin?Elsner Michael?Berg Rainer?U?Meckenstock Stefan?B?Haderlein |
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Institution: | (1) Environmental Mineralogy, Center for Applied Geoscience, Eberhard-Karls-University Tübingen, Wilhelmstr. 56, 72074 Tübingen, Germany;(2) Swiss Federal Institute for Environmental Science and Technology (EAWAG), Ueberlandstr. 133, 8600 Dübendorf, Switzerland;(3) Present address: Institute for Hydrology, GSF-Research Center for Environment and Health, Ingolstädter Landstr. 1, 85764 Neuherberg, Germany |
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Abstract: | Compound-specific stable isotope analysis (CSIA) using gas chromatography-isotope ratio mass spectrometry (GC/IRMS) has developed into a mature analytical method in many application areas over the last decade. This is in particular true for carbon isotope analysis, whereas measurements of the other elements amenable to CSIA (hydrogen, nitrogen, oxygen) are much less routine. In environmental sciences, successful applications to date include (i) the allocation of contaminant sources on a local, regional, and global scale, (ii) the identification and quantification of (bio)transformation reactions on scales ranging from batch experiments to contaminated field sites, and (iii) the characterization of elementary reaction mechanisms that govern product formation. These three application areas are discussed in detail. The investigated spectrum of compounds comprises mainly n-alkanes, monoaromatics such as benzene and toluene, methyl tert-butyl ether (MTBE), polycyclic aromatic hydrocarbons (PAHs), and chlorinated hydrocarbons such as tetrachloromethane, trichloroethylene, and polychlorinated biphenyls (PCBs). Future research directions are primarily set by the state of the art in analytical instrumentation and method development. Approaches to utilize HPLC separation in CSIA, the enhancement of sensitivity of CSIA to allow field investigations in the µg L–1 range, and the development of methods for CSIA of other elements are reviewed. Furthermore, an alternative scheme to evaluate isotope data is outlined that would enable estimates of position-specific kinetic isotope effects and, thus, allow one to extract mechanistic chemical and biochemical information.Abbreviations BTEX
benzene, toluene, ethylbenzene, xylenes
- MTBE
methyl tert-butyl ether
- PAHs
polycyclic aromatic hydrocarbons
- VOCs
volatile compounds
- PCBs
polychlorinated biphenyls
- CSIA
compound-specific (stable) isotope (ratio) analysis
- GC-IRMS, GC/IRMS or GCIRMS
gas chromatography-isotope ratio mass spectrometry
- GC-C-IRMS, GC/C/IRMS or GCC-IRMS
gas chromatography-combustion-isotope ratio mass spectrometry
- irmGC/MS
isotope ratio monitoring gas chromatograph-mass spectrometry
- GC/P/IRMS
gas chromatography-pyrolysis-isotope ratio mass spectrometry (used for D/H)
- KIE
kinetic isotope effect
- PSIA
position-specific isotope analysis (for intramolecular isotope distribution)
- SNIF-NMR
site-specific natural isotopic fractionation by nuclear magnetic resonance spectroscopy |
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Keywords: | CSIA IRMS Isotope fractionation Isotope ratio Isotopic shift Fingerprinting Source allocation Biodegradation Degradation Transformation Weathering Environmental forensics Geomicrobiology Contaminant hydrology SPME Purge and trap 13C D/H Primary isotope effect Secondary isotope effect Kinetic isotope effect Rayleigh equation Chloromethane Tetrachloromethane Trichloroethylene Tetrachloroethylene Methane Perylene Creosote Sulfate Chlorinated solvents PAH PCB Aromatic hydrocarbon Biogenic Petrogenic BTEX VOC |
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